WO2017056684A1 - Organic electroluminescence panel and production method therefor - Google Patents

Organic electroluminescence panel and production method therefor Download PDF

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WO2017056684A1
WO2017056684A1 PCT/JP2016/072556 JP2016072556W WO2017056684A1 WO 2017056684 A1 WO2017056684 A1 WO 2017056684A1 JP 2016072556 W JP2016072556 W JP 2016072556W WO 2017056684 A1 WO2017056684 A1 WO 2017056684A1
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organic
light
layer
anode
light emitting
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PCT/JP2016/072556
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French (fr)
Japanese (ja)
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一由 小俣
司 八木
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コニカミノルタ株式会社
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Priority to US15/759,689 priority Critical patent/US20190044091A1/en
Priority to JP2017542973A priority patent/JPWO2017056684A1/en
Publication of WO2017056684A1 publication Critical patent/WO2017056684A1/en

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    • H—ELECTRICITY
    • H10—SEMICONDUCTOR DEVICES; ELECTRIC SOLID-STATE DEVICES NOT OTHERWISE PROVIDED FOR
    • H10K—ORGANIC ELECTRIC SOLID-STATE DEVICES
    • H10K50/00—Organic light-emitting devices
    • H10K50/80—Constructional details
    • H10K50/805—Electrodes
    • H10K50/81—Anodes
    • H—ELECTRICITY
    • H10—SEMICONDUCTOR DEVICES; ELECTRIC SOLID-STATE DEVICES NOT OTHERWISE PROVIDED FOR
    • H10K—ORGANIC ELECTRIC SOLID-STATE DEVICES
    • H10K50/00—Organic light-emitting devices
    • H10K50/80—Constructional details
    • H10K50/805—Electrodes
    • H10K50/82—Cathodes
    • H10K50/828—Transparent cathodes, e.g. comprising thin metal layers
    • H—ELECTRICITY
    • H10—SEMICONDUCTOR DEVICES; ELECTRIC SOLID-STATE DEVICES NOT OTHERWISE PROVIDED FOR
    • H10K—ORGANIC ELECTRIC SOLID-STATE DEVICES
    • H10K59/00—Integrated devices, or assemblies of multiple devices, comprising at least one organic light-emitting element covered by group H10K50/00
    • H10K59/80—Constructional details
    • H10K59/86—Series electrical configurations of multiple OLEDs
    • H—ELECTRICITY
    • H10—SEMICONDUCTOR DEVICES; ELECTRIC SOLID-STATE DEVICES NOT OTHERWISE PROVIDED FOR
    • H10K—ORGANIC ELECTRIC SOLID-STATE DEVICES
    • H10K71/00—Manufacture or treatment specially adapted for the organic devices covered by this subclass
    • H—ELECTRICITY
    • H10—SEMICONDUCTOR DEVICES; ELECTRIC SOLID-STATE DEVICES NOT OTHERWISE PROVIDED FOR
    • H10K—ORGANIC ELECTRIC SOLID-STATE DEVICES
    • H10K71/00—Manufacture or treatment specially adapted for the organic devices covered by this subclass
    • H10K71/20—Changing the shape of the active layer in the devices, e.g. patterning
    • H10K71/231—Changing the shape of the active layer in the devices, e.g. patterning by etching of existing layers
    • H10K71/233—Changing the shape of the active layer in the devices, e.g. patterning by etching of existing layers by photolithographic etching
    • H—ELECTRICITY
    • H10—SEMICONDUCTOR DEVICES; ELECTRIC SOLID-STATE DEVICES NOT OTHERWISE PROVIDED FOR
    • H10K—ORGANIC ELECTRIC SOLID-STATE DEVICES
    • H10K2102/00—Constructional details relating to the organic devices covered by this subclass
    • H—ELECTRICITY
    • H10—SEMICONDUCTOR DEVICES; ELECTRIC SOLID-STATE DEVICES NOT OTHERWISE PROVIDED FOR
    • H10K—ORGANIC ELECTRIC SOLID-STATE DEVICES
    • H10K2102/00—Constructional details relating to the organic devices covered by this subclass
    • H10K2102/301—Details of OLEDs
    • H10K2102/302—Details of OLEDs of OLED structures
    • H10K2102/3023—Direction of light emission
    • H10K2102/3031—Two-side emission, e.g. transparent OLEDs [TOLED]
    • H—ELECTRICITY
    • H10—SEMICONDUCTOR DEVICES; ELECTRIC SOLID-STATE DEVICES NOT OTHERWISE PROVIDED FOR
    • H10K—ORGANIC ELECTRIC SOLID-STATE DEVICES
    • H10K2102/00—Constructional details relating to the organic devices covered by this subclass
    • H10K2102/301—Details of OLEDs
    • H10K2102/311—Flexible OLED
    • H—ELECTRICITY
    • H10—SEMICONDUCTOR DEVICES; ELECTRIC SOLID-STATE DEVICES NOT OTHERWISE PROVIDED FOR
    • H10K—ORGANIC ELECTRIC SOLID-STATE DEVICES
    • H10K2102/00—Constructional details relating to the organic devices covered by this subclass
    • H10K2102/301—Details of OLEDs
    • H10K2102/351—Thickness
    • H—ELECTRICITY
    • H10—SEMICONDUCTOR DEVICES; ELECTRIC SOLID-STATE DEVICES NOT OTHERWISE PROVIDED FOR
    • H10K—ORGANIC ELECTRIC SOLID-STATE DEVICES
    • H10K50/00—Organic light-emitting devices
    • H10K50/80—Constructional details
    • H10K50/84—Passivation; Containers; Encapsulations
    • H10K50/844—Encapsulations
    • H—ELECTRICITY
    • H10—SEMICONDUCTOR DEVICES; ELECTRIC SOLID-STATE DEVICES NOT OTHERWISE PROVIDED FOR
    • H10K—ORGANIC ELECTRIC SOLID-STATE DEVICES
    • H10K59/00—Integrated devices, or assemblies of multiple devices, comprising at least one organic light-emitting element covered by group H10K50/00
    • H10K59/10—OLED displays
    • H—ELECTRICITY
    • H10—SEMICONDUCTOR DEVICES; ELECTRIC SOLID-STATE DEVICES NOT OTHERWISE PROVIDED FOR
    • H10K—ORGANIC ELECTRIC SOLID-STATE DEVICES
    • H10K77/00—Constructional details of devices covered by this subclass and not covered by groups H10K10/80, H10K30/80, H10K50/80 or H10K59/80
    • H10K77/10—Substrates, e.g. flexible substrates
    • H10K77/111—Flexible substrates

Definitions

  • the present invention relates to a light-transmitting organic electroluminescence panel applied to various display devices (hereinafter, also referred to as “displays”), lighting devices, and the like, and more specifically, the present invention relates to light transmission.
  • TECHNICAL FIELD The present invention relates to an organic electroluminescence panel in which a plurality of light emitting areas composed of organic electroluminescence elements having a property are arranged, a wide light emitting area, and brightness uniformity and stability are improved, and a method for manufacturing the same.
  • organic electroluminescence L element (hereinafter abbreviated as “organic EL element”) using an organic material electroluminescence (hereinafter abbreviated as “EL”) has a voltage of about several V to several tens of volts. It is a thin-film, completely solid element that can emit light at a low voltage, and has many excellent features such as high brightness, high luminous efficiency, thinness, and light weight. For this reason, organic EL elements have attracted attention in recent years as surface light emitters such as backlights for various displays, smart devices, and illumination light sources.
  • Such an organic EL element has a structure in which a light emitting layer made of an organic material is sandwiched between two opposing electrodes, and light emitted from the light emitting layer is transmitted through the electrode and taken out to the outside. For this reason, at least one of the two electrodes is configured as a light-transmitting electrode (hereinafter also referred to as a transparent electrode).
  • an oxide semiconductor material such as indium tin oxide (SnO 2 —In 2 O 3 : Indium Tin Oxide, hereinafter abbreviated as “ITO”) is generally used. ing.
  • both the anode and the cathode are composed of a transparent electrode pair having light transmittance across the light emitting layer, and as such a light transmitting electrode,
  • ITO was generally used.
  • the performance as an anode was excellent, but the performance as a cathode tended to be inferior.
  • a display electrode having a light transmitting property using electrodes having a light transmitting property on both sides in order to obtain high performance with the current technology, both the anode and the cathode are not ITO-ITO electrodes.
  • a light-transmitting display in which an electrode such as anode ITO-cathode aluminum is used and a light-emitting portion and a see-through portion (light transmission portion) are provided by minimizing the area of the cathode (for example, Patent Document 1). reference.).
  • a light-transmitting electrode composed of silver having a high electrical conductivity or an alloy of silver and aluminum is known as a cathode.
  • the anode and the cathode Many of the thin film metal layers and oxide semiconductors used have a high resistance value and a large voltage drop.
  • the light-transmitting electrode is made thin, or the light emitting area of the element is reduced. If the area is increased, the sheet resistance value will increase and the luminance uniformity will be greatly reduced. This will be a major obstacle to the development of organic electroluminescence devices that aim to increase the area and brightness in the future. It has become.
  • the cause of uneven brightness due to the increase in area is that by increasing the size of the light emitting screen, there are places where a large amount of current flows and places where only a small amount of current flows in the screen. Arise. Since the luminance of the organic EL element increases as the flowing current increases, the presence of a portion where a large amount of current flows and a portion where a small amount of current flows causes a difference in luminance between the two, which causes luminance unevenness.
  • a life difference occurs in each light emitting region in the organic EL element as the size increases. This is because the lifetime of the organic EL element is changed between a portion where a large amount of current flows and a portion where a small amount of current flows. In general, the life of a portion where a large amount of current flows is shortened. For this reason, as compared with an element in which current flows uniformly, a portion having a short lifetime exists, and the lifetime as an organic EL element is shortened.
  • Japanese Patent Laid-Open No. 5-315073 discloses a technique of providing a plurality of voltage application extraction portions (the terminal portions).
  • the size of a device such as a portable terminal in which the organic EL element is incorporated is limited
  • the size of the organic EL element is also limited. That is, in order to increase the light emitting area of the organic EL element, the total area of the terminal portion must be reduced.
  • an organic EL device having a structure in which a plurality of light emitting regions are provided, an insulating portion is provided between light-transmitting electrodes of physically adjacent light emitting regions, and the plurality of light emitting regions are electrically connected in series.
  • a transparent organic EL element comprising a first transparent electrode, an insulating partition, an organic EL layer and a second transparent electrode divided by the partition on a transparent substrate is disclosed (for example, a patent) Reference 4).
  • the resistance of the second transparent electrode layer can be reduced without causing a short circuit even if the alignment is shifted.
  • the current value in each organic EL element becomes high, causing non-uniformity of light emission, and when used under harsh conditions, cutting the wiring connecting each electrode or short-circuiting between the electrodes It turned out to be easy to cause.
  • the present invention has been made in view of the above problems, and a solution to the problem is a wide light-emitting area that is composed of a light-transmitting organic electroluminescence element and is composed of a plurality of divided light-emitting areas.
  • Another object of the present invention is to provide an organic electroluminescence panel having improved luminance uniformity and stability and a method for manufacturing the same.
  • the present inventor has an organic electroluminescent element having a double-sided light-transmitting property, and the organic electroluminescent element has at least a light transmitting property on a substrate.
  • a light emitting area composed of an anode having an organic functional layer unit and a light-transmitting cathode is divided into a plurality of parts, and the cathode is separated by a separator provided on the anode, and one light emitting area
  • the organic electroluminescence panel is characterized in that the anode constituting the light-emitting element is electrically connected in series with the cathode constituting the other light-emitting area.
  • An organic electroluminescence panel with improved brightness uniformity and stability can be realized. Found that it is, it has led to the present invention.
  • An organic electroluminescence panel having an organic electroluminescence element having a light transmittance of 50% or more at a wavelength of 550 nm when not emitting light
  • a light emitting area composed of at least an anode, an organic functional layer unit, and a cathode is divided into a plurality of parts on a base material,
  • the anode and the cathode constituting the light emitting area are both composed of electrodes having light transmittance,
  • the cathode is separated by a separator provided on the anode,
  • An organic electroluminescence panel wherein an anode constituting one of the divided light emitting areas is electrically connected in series with a cathode constituting the other adjacent light emitting area.
  • the light-transmitting cathode has an underlayer composed of a nitrogen-containing compound and an electrode layer composed of silver or an alloy containing silver as a main component on the underlayer.
  • the organic electroluminescence panel according to any one of items 1 to 6, wherein:
  • a manufacturing method of the organic electroluminescent panel which manufactures the organic electroluminescent panel as described in any one of Claim 1 to 11, Having an organic electroluminescence device having a light transmittance of 50% or more at a wavelength of 550 nm when not emitting light,
  • a light emitting area composed of at least an anode, an organic functional layer unit and a cathode is divided into a plurality of parts, Forming a pattern in which the cathode is separated by a separator provided on the anode;
  • the anode constituting one light emitting area that is divided is electrically connected in series with the cathode constituting the other neighboring light emitting area, And the said anode, a cathode, and a separator are formed by the photolithographic method,
  • the manufacturing method of the organic electroluminescent panel characterized by the above-mentioned.
  • an organic electroluminescence panel having a wide light emitting area composed of a plurality of divided light emitting areas and having improved luminance uniformity and stability, and a method for manufacturing the same.
  • the light emitting area is divided into a plurality of parts (the number of divisions is N), and the anode constituting one light emitting area is electrically connected in series with the cathode constituting the other light emitting area.
  • the required current is reduced to I / N, so that the voltage drop of the anode or cathode from the feed end to the center of the panel is also reduced to I / N.
  • the organic electroluminescence panel of the present invention has an organic electroluminescence element having a light transmittance of 50% or more at a wavelength of 550 nm when not emitting light, and the organic electroluminescence element has at least an anode and an organic function on a substrate.
  • a light emitting area composed of a layer unit and a cathode is divided into a plurality of parts, each of the anode and the cathode constituting the light emitting area is composed of a light-transmitting electrode, and the cathode is the anode.
  • an insulating layer is further provided between the anode and the separator in the same light emitting area. This is a preferable form from the viewpoint that the insulation between the electrodes can be further improved and the stability can be further improved.
  • a gas barrier layer is formed between the flexible resin base material and the organic EL constituent layer due to moisture, oxygen, or the like with respect to the organic EL constituent layer. It is preferable from the viewpoint that the influence can be eliminated and high durability can be obtained.
  • the light-transmitting anode is made of an oxide semiconductor or a thin-film metal or alloy because an electrode having both high light transmittance and excellent conductivity can be obtained.
  • the light-transmitting cathode is composed of at least a thin metal or alloy because an electrode having both high light transmittance and excellent conductivity can be obtained.
  • an electrode layer made of silver or an alloy containing silver as a main component is applied as a light-transmitting cathode, a base layer made of a nitrogen-containing compound is provided, and the electrode is formed on the upper layer. It is preferable to form a layer from the viewpoint that, as a cathode, silver atoms are present without causing aggregation or the like, and a uniform thin silver film can be formed.
  • the connecting portion between the organic electroluminescence panel and the external electrode is electrically connected by a conductive adhesive.
  • the fact that a plurality of organic electroluminescence elements are sealed with a flexible resin substrate having a gas barrier layer can eliminate the influence of moisture, oxygen, etc. on the organic EL constituent layer, and has high durability. From the viewpoint that can be obtained.
  • a plurality of light emitting areas are arranged in parallel in a stripe shape from the viewpoint of obtaining stable light emission characteristics by efficiently dividing a large area.
  • the external electrode is composed of a light-transmitting flexible printed circuit from the viewpoint of being able to design a thin film and highly light-transmitting circuit.
  • the organic electroluminescent panel of this invention has the organic electroluminescent element which is 50% or more of the light transmittance in wavelength 550nm at the time of the non-light-emitting which consists of a structure prescribed
  • the said organic electroluminescent In the element a light emitting area composed of at least an anode, an organic functional layer unit, and a cathode is formed on a substrate by dividing it into a plurality, and a pattern is formed in which the cathode is separated by a separator provided on the anode.
  • the anode constituting one of the divided light emitting areas is electrically connected in series with the cathode constituting the other neighboring light emitting area, and the anode, the cathode and the separator are connected by photolithography.
  • the manufacturing method of the organic electroluminescent panel characterized by forming Rukoto is possible to form a structure pattern with high precision, it is possible to manufacture an organic electroluminescent panel capable of forming a narrow non-light emitting area.
  • an insulating layer using a photolithography method between the anode and the separator in that a high insulating property can be obtained and a high-definition insulating layer can be formed. It is.
  • the “organic EL panel” refers to a plurality of organic EL elements constituting a light emitting area divided into a plurality of parts arranged in the same plane, and the anode of the organic EL element is electrically connected to the other adjacent cathode. In contact with each other and constituting a large-area light emitter.
  • the “organic EL element” as used in the present invention is an element that constitutes a divided light-emitting area, and has a pair of opposed light-transmitting electrodes (anode and cathode) on the base material and the light-transmitting property.
  • description and description of the sealing member may be omitted for convenience of explanation.
  • description of a control circuit and wiring for controlling light emission of the organic EL element is omitted.
  • a first carrier transporting functional layer group 1 for example, a hole injection layer, a hole is formed on a substrate.
  • a transport layer, a light emitting layer containing a phosphorescent compound, and the like, and a second carrier transport function layer group 2 for example, a hole blocking layer, an electron transport layer, an electron injection layer, and the like. Refers to the configuration.
  • the “light emitting area” refers to a region where all components of the anode, the organic functional layer unit, and the cathode exist in the layer thickness direction.
  • the “anode” is an electrode to which (+) is applied as a voltage, and may be referred to as “anode” or “first electrode”.
  • the “cathode” is an electrode to which ( ⁇ ) is applied as a voltage, and may be referred to as “cathode” or “second electrode”.
  • the “light transmittance” in the present invention means that the light transmittance at a wavelength of 550 nm is 50% or more, preferably 60% or more, and more preferably 70% or more.
  • the applied organic EL element is a double-sided light emitting organic EL element having a light transmittance of 50% or more at a wavelength of 550 nm when not emitting light.
  • FIG. 1 is a schematic sectional view showing a basic configuration including an organic functional layer unit of an organic EL element applicable to the present invention.
  • the organic EL element (OLED) according to the present invention shown in FIG. 1 is formed on a light-transmitting substrate (1) such as a glass substrate or a flexible resin substrate, an anode (3), a light emitting layer, and a carrier.
  • a light-transmitting substrate (1) such as a glass substrate or a flexible resin substrate, an anode (3), a light emitting layer, and a carrier.
  • a structure in which an organic functional layer unit (U) composed of a transport functional layer, a cathode (7), and the like are laminated is shown.
  • the organic EL element (OLED) shown in FIG. 1 shows an example in which a gas barrier layer (2) is formed on a light-transmitting substrate (1).
  • the anode (3) is formed as the first electrode, and on the upper part of one end (left side in FIG. 1) of the anode (3), A separator (8) is provided.
  • This separator (8) may be called a partition or a cathode separator.
  • the organic functional layer unit (U) is configured by laminating the layer (5) and the second carrier transport functional layer group 2 (6) composed of, for example, an electron transport layer, an electron injection layer, and the like.
  • a cathode (7) is provided as a second electrode between the separators (8) of one organic EL element (OLED) and the other adjacent organic EL element in an independent pattern.
  • substrate (11) which has the contact bonding layer (9) and a gas barrier layer (10) is provided in the form which coat
  • the anode (3) constituting one divided light emitting area is electrically connected in series with the cathode (3) constituting the other adjacent light emitting area.
  • the anode (3) as the first electrode and the cathode (7) as the second electrode are both electrodes having a light transmittance of 50% or more at a wavelength of 550 nm. This is one feature.
  • the emitted light (L) emitted from the light emitting layer of the organic functional layer unit or its interface is used as the first electrode having optical transparency.
  • the emitted light (L) is emitted from the light emitting area on the substrate (1) surface which is the side and the light emitting area on the sealing electrode (11) side on the second electrode (7) side which is also light transmissive. Can be taken out.
  • the light emitting area means that all components of the anode (3), the organic functional layer unit (U), particularly the light emitting layer (5), and the cathode (7) are on the same plane. An area that exists.
  • a plurality of light-emitting areas composed of at least the anode (8), the organic functional layer unit (U), and the cathode (7) are provided on the substrate via the separator (8).
  • the anodes that are divided and arranged so that one of the divided light emitting areas is electrically connected in series with the cathode that constitutes the other adjacent light emitting area. . Specifically, as shown in FIG.
  • an anode (3) constituting an organic EL element (OLED) shown as “one constituent unit of OLED” is disposed on the left side (detailed description is omitted) (7 ) And the cathode (7) of the organic EL element (OLED) shown as “one constituent unit of OLED” is arranged on the right side (detailed configuration is omitted).
  • the organic EL element according to the present invention may have a tandem configuration in which two or more organic functional layer units are stacked.
  • the light emitting area is divided into a plurality of parts via the separator (8), and the anode constituting one of the divided light emitting areas is used as the other adjacent light emitting area.
  • the cathode By configuring the cathode to be electrically connected in series, the current value required for light emission was reduced, and a large-area organic EL panel excellent in luminance uniformity could be realized.
  • the light-transmitting organic EL element (OLED) according to the present invention overlaps with the description in FIG. 1 described above, but the light transmission as the first electrode on the substrate (1) having the gas barrier layer (2).
  • the anode (3) having the property is formed as a first electrode in a region divided on the gas barrier layer (2), and one end of the anode (3) (the left side in FIG. 1) ) Is provided with an inverted trapezoidal separator (8).
  • a carrier transport function layer group 1 (4) composed of a hole injection layer, a hole transport layer, and the like, a light emitting layer (5)
  • a carrier transport functional layer group 2 (6) composed of an electron transport layer, an electron injection layer, and the like is laminated to form a light emitting region.
  • a light-transmitting cathode (7) as a second electrode is formed in a region separated by the pair of upper separators (8), and a sealing adhesive layer (9) and a gas are formed thereon.
  • a sealing substrate (11) having a barrier layer (10) is provided.
  • tandem organic EL element can also be used.
  • tandem type include, for example, US Pat. No. 6,337,492, US Pat. No. 7,420,203, US Pat. No. 7,473,923, US Pat. No. 6,872,472, US Pat. No. 6,107,734, US Pat. No. 6,337,492, WO 2005/009087, JP 2006-228712, JP 2006-24791, JP 2006- No. 49393, JP-A-2006-49394, JP-A-2006-49396, JP-A-2011-96679, JP-A-2005-340187, JP-A-4711424, JP-A-3496681, Patent No. No. 3884564, Japanese Patent No.
  • the substrate (1) applicable to the organic EL element (OLED) is not particularly limited as long as it is a light-transmitting substrate, and examples thereof include glass and resin substrates.
  • Examples of the light-transmitting substrate (1) applicable to the present invention include glass, quartz, and a resin substrate. More preferably, the organic EL element can be provided with flexibility. To flexible resin base material.
  • polyesters such as polyethylene terephthalate (abbreviation: PET), polyethylene naphthalate (abbreviation: PEN), polyethylene, polypropylene, cellophane, cellulose diacetate, and cellulose.
  • Cellulose esters such as triacetate (abbreviation: TAC), cellulose acetate butyrate, cellulose acetate propionate (abbreviation: CAP), cellulose acetate phthalate, cellulose nitrate, and their derivatives, polyvinylidene chloride, polyvinyl alcohol, polyethylene vinyl alcohol , Syndiotactic polystyrene, polycarbonate (abbreviation: PC), norbornene resin, polymethylpentene, polyetherketone, polyimide, Ether sulfone (abbreviation: PES), polyphenylene sulfide, polysulfones, polyether imide, polyether ketone imide, polyamide, fluororesin, nylon, polymethyl methacrylate, acrylic and polyarylates, Arton (trade name, manufactured by JSR) and Examples thereof include cycloolefin resins such as Apel (trade name, manufactured by Mitsui Chemicals).
  • TAC triacetate
  • polyethylene terephthalate (abbreviation: PET), polybutylene terephthalate, polyethylene naphthalate (abbreviation: PEN), polycarbonate (abbreviation: PC), etc.
  • PET polyethylene terephthalate
  • PEN polyethylene naphthalate
  • PC polycarbonate
  • a resin base material can be preferably used.
  • the resin substrate may be an unstretched film or a stretched film.
  • the resin base material applicable to the present invention can be manufactured by a conventionally known film forming method.
  • an unstretched resin base material that is substantially amorphous and not oriented can be produced by melting a resin as a material with an extruder, extruding it with an annular die or a T-die, and quenching.
  • a resin substrate produced by a solution casting method in which a resin component is dissolved in a solvent to prepare a dope and then the dope is cast on a metal support and dried to form a film can also be applied.
  • the unstretched resin base material is transported in the direction of the resin base material (vertical axis direction) by a known method such as uniaxial stretching, tenter sequential biaxial stretching, tenter simultaneous biaxial stretching, tubular simultaneous biaxial stretching, or the like. , MD direction), or a stretched resin substrate can be produced by stretching in a direction perpendicular to the conveying direction of the resin substrate (horizontal axis direction, TD direction).
  • the draw ratio in this case can be appropriately selected according to the resin as the raw material of the resin base material, but is preferably in the range of 1.01 to 10 times in the vertical axis direction and the horizontal axis direction.
  • the resin substrate is preferably a thin film resin substrate having a thickness in the range of 3 to 200 ⁇ m, more preferably in the range of 10 to 150 ⁇ m, and particularly preferably in the range of 20 to 120 ⁇ m. It is.
  • the light-transmitting anode constituting the organic EL element is preferably composed of an oxide semiconductor or a thin-film metal or alloy, for example, a metal such as Ag or Au or a metal as a main component.
  • oxide semiconductors such as CuI, indium-tin composite oxide (ITO), SnO 2 and ZnO.
  • the purity of silver is preferably 99% or more. Further, palladium (Pd), copper (Cu), gold (Au), or the like may be added to ensure the stability of silver.
  • the light-transmitting anode can be a layer composed mainly of silver.
  • the anode can be formed of silver alone or an alloy containing silver (Ag). It may be.
  • alloys include silver / magnesium (Ag / Mg), silver / copper (Ag / Cu), silver / palladium (Ag / Pd), silver / palladium / copper (Ag / Pd / Cu), silver -Indium (Ag.In) etc. are mentioned.
  • an anode having a light transmission property composed mainly of silver and having a thickness in the range of 2 to 20 nm.
  • the thickness is preferably in the range of 4 to 12 nm.
  • a thickness of 20 nm or less is preferable because the absorption component and reflection component of the light-transmitting anode are kept low and high light transmittance is maintained.
  • the layer composed mainly of silver in the present invention means that the silver content in the light-transmitting anode is 60% by mass or more, preferably the silver content is 80% by mass. More preferably, the silver content is 90% by mass or more, and particularly preferably the silver content is 98% by mass or more.
  • “light transmittance” in the anode having light transmittance according to the present invention means that the light transmittance at a wavelength of 550 nm is 50% or more.
  • the light-transmitting anode may have a structure in which a layer composed mainly of silver is divided into a plurality of layers as necessary.
  • the lower portion is formed from the viewpoint of improving the uniformity of the silver film of the light-transmitting anode to be formed.
  • an underlayer it is a layer containing the organic compound which has a nitrogen atom or a sulfur atom, and forms the anode which has a light transmittance which has silver as a main component on the said base layer.
  • the method is a preferred embodiment. The details of the underlayer applicable to the present invention will be described later.
  • the present invention is characterized in that a separator is provided between each organic EL element, and the cathode is separated by two separators provided on the anode.
  • the separator according to the present invention is formed in a stripe shape in a direction perpendicular to the longitudinal direction of the anode.
  • This separator has an insulating property and has a function of dividing the cathode into a plurality of areas.
  • the separator is also formed in a stripe shape so as to be orthogonal to the longitudinal direction of the stripe-shaped anode.
  • the cathode can be divided into a plurality of areas. Therefore, the cross-sectional shape of the separator is not particularly limited. For example, a rectangular shape, a trapezoidal shape (in order) Taper shape), reverse taper shape and the like. A reverse taper overhang structure as shown in FIG. 1 is preferable.
  • the taper angle ⁇ with respect to the substrate or the anode surface may be 0 ° ⁇ ⁇ 90 °, preferably 20 ° ⁇ ⁇ 80 °, more preferably 30 ° ⁇ ⁇ . 70 °.
  • the height from the surface of the anode or the insulating layer, which is the base of the separator, to the surface of the separator is usually higher than the height from the surface of the substrate (1) to the surface of the cathode (7) at the center of the light emitting region. Is set to be higher.
  • the width of the separator is not particularly limited, but is preferably 100 ⁇ m or less. If the width of the separator is too wide, the light emitting region becomes relatively narrow and the light emitting area is reduced, which is not preferable.
  • the pitch of the separator is not particularly limited, and is appropriately selected depending on the pixel size of the target organic EL element.
  • a photosensitive polyimide resin for example, a photosensitive polyimide resin, an acrylic resin, a novolac resin, a styrene resin, a phenol resin, a photocurable resin such as a melamine resin, or a thermosetting resin, an inorganic material, etc.
  • an acrylic resin for example, acrylic resin, a novolac resin, a styrene resin, a phenol resin, a photocurable resin such as a melamine resin, or a thermosetting resin, an inorganic material, etc.
  • Examples of the method for forming the separator include general methods such as a photolithography method and a printing method.
  • the separator is formed by a photolithography method. . Details of the method for forming the separator by photolithography will be described later.
  • a phosphorescent light emitting compound or a fluorescent compound can be used as the light emitting material.
  • a phosphorescent light emitting compound is used as the light emitting material.
  • the contained structure is preferable.
  • This light emitting layer is a layer that emits light by recombination of electrons injected from the electrode or the electron transport layer and holes injected from the hole transport layer, and the light emitting portion is an in-layer region of the light emitting layer. Even the interface region between the light emitting layer and the adjacent layer may be used.
  • Such a light emitting layer is not particularly limited in its configuration as long as the light emitting material contained satisfies the light emission requirements. Moreover, there may be a plurality of layers having the same emission spectrum and emission maximum wavelength. In this case, it is preferable to have a non-light emitting intermediate layer between the light emitting layers.
  • the total thickness of the light emitting layers is preferably in the range of 1 to 100 nm, and more preferably in the range of 1 to 30 nm because a lower driving voltage can be obtained.
  • the sum total of the thickness of a light emitting layer is the thickness also including the said intermediate
  • the light emitting layer as described above is prepared by using a known method such as a vacuum evaporation method, a spin coating method, a casting method, an LB method (Langmuir-Blodget, Langmuir Blodgett method) and an ink jet method. Can be formed.
  • a known method such as a vacuum evaporation method, a spin coating method, a casting method, an LB method (Langmuir-Blodget, Langmuir Blodgett method) and an ink jet method. Can be formed.
  • a plurality of light emitting materials may be mixed, and a phosphorescent light emitting material and a fluorescent light emitting material (also referred to as a fluorescent dopant or a fluorescent compound) may be mixed and used in the same light emitting layer.
  • the structure of the light-emitting layer preferably includes a host compound (also referred to as a light-emitting host) and a light-emitting material (also referred to as a light-emitting dopant compound), and emits light from the light-emitting material.
  • ⁇ Host compound> As the host compound contained in the light emitting layer, a compound having a phosphorescence quantum yield of phosphorescence emission at room temperature (25 ° C.) of less than 0.1 is preferable. Further, the phosphorescence quantum yield is preferably less than 0.01. Moreover, it is preferable that the volume ratio in the layer is 50% or more among the compounds contained in a light emitting layer.
  • the host compound a known host compound may be used alone, or a plurality of types of host compounds may be used. By using a plurality of types of host compounds, it is possible to adjust the movement of charges, and the organic EL element can be made highly efficient. In addition, by using a plurality of kinds of light emitting materials described later, it is possible to mix different light emission, thereby obtaining an arbitrary light emission color.
  • the host compound used in the light emitting layer may be a conventionally known low molecular compound or a high molecular compound having a repeating unit, and a low molecular compound having a polymerizable group such as a vinyl group or an epoxy group (evaporation polymerizable light emitting host). )
  • Examples of host compounds applicable to the present invention include, for example, JP-A Nos. 2001-257076, 2001-357777, 2002-8860, 2002-43056, 2002-105445, 2002-352957, 2002-231453, 2002-234888, 2002-260861, 2002-305083, US Patent Application Publication No. 2005/0112407, US Patent Application Publication No. 2009/0030202, International Publication No. 2001/039234, International Publication No. 2008/056746, International Publication No. 2005/089025, International Publication No. 2007/063754, International Publication No. 2005/030900, International Publication 200th / No. 086,028, WO 2012/023947, can be mentioned JP 2007-254297, JP-European compounds described in Japanese Patent No. 2034538 Pat like.
  • a phosphorescent compound also referred to as a phosphorescent compound, a phosphorescent material, or a phosphorescent dopant
  • a fluorescent compound both a fluorescent compound or a fluorescent material
  • a phosphorescent compound is a compound in which light emission from an excited triplet is observed. Specifically, it is a compound that emits phosphorescence at room temperature (25 ° C.), and the phosphorescence quantum yield is 0 at 25 ° C.
  • a preferred phosphorescence quantum yield is 0.1 or more, although it is defined as 0.01 or more compounds.
  • the phosphorescent quantum yield can be measured by the method described in Spectroscopic II, page 398 (1992 edition, Maruzen) of the Fourth Edition Experimental Chemistry Course 7.
  • the phosphorescence quantum yield in the solution can be measured using various solvents, but when using a phosphorescent compound in the present invention, the phosphorescence quantum yield is 0.01 or more in any solvent. Should be achieved.
  • the phosphorescent compound can be appropriately selected from known compounds used for the light-emitting layer of a general organic EL device, but preferably contains a group 8 to 10 metal in the periodic table of elements. More preferred are iridium compounds, more preferred are iridium compounds, osmium compounds, platinum compounds (platinum complex compounds) or rare earth complexes, and most preferred are iridium compounds.
  • At least one light emitting layer may contain two or more phosphorescent compounds, and the concentration ratio of the phosphorescent compound in the light emitting layer varies in the thickness direction of the light emitting layer. It may be an embodiment.
  • preferred phosphorescent compounds include organometallic complexes having Ir as a central metal. More preferably, a complex containing at least one coordination mode of a metal-carbon bond, a metal-nitrogen bond, a metal-oxygen bond, and a metal-sulfur bond is preferable.
  • the phosphorescent compound described above (also referred to as a phosphorescent metal complex) is described in, for example, Organic Letter, vol. 16, 2579-2581 (2001), Inorganic Chemistry, Vol. 30, No. 8, pp. 1685-1687 (1991), J. Am. Am. Chem. Soc. , 123, 4304 (2001), Inorganic Chemistry, Vol. 40, No. 7, pages 1704-1711 (2001), Inorganic Chemistry, Vol. 41, No. 12, pages 3055-3066 (2002) , New Journal of Chemistry. 26, 1171 (2002), European Journal of Organic Chemistry, Vol. 4, pages 695-709 (2004), and methods disclosed in the references and the like described in these documents Can be synthesized.
  • Fluorescent compounds include coumarin dyes, pyran dyes, cyanine dyes, croconium dyes, squalium dyes, oxobenzanthracene dyes, fluorescein dyes, rhodamine dyes, pyrylium dyes, perylene dyes, stilbene dyes. And dyes, polythiophene dyes, and rare earth complex phosphors.
  • Carrier transport functional group Next, a charge injection layer, a hole transport layer, an electron transport layer, and a blocking layer will be described in this order as representative examples of the layers constituting the carrier transport functional layer group.
  • the charge injection layer is a layer provided between the electrode and the light emitting layer in order to lower the driving voltage and improve the light emission luminance.
  • the organic EL element and its industrialization front line June 30, 1998, NT. The details are described in Volume 2, Chapter 2, “Electrode Materials” (pages 123 to 166) of “Part 2” of S Co., Ltd., and there are a hole injection layer and an electron injection layer.
  • the charge injection layer is present between the anode and the light emitting layer or the hole transport layer in the case of a hole injection layer, and between the cathode and the light emitting layer or the electron transport layer in the case of an electron injection layer.
  • the hole injection layer is a layer disposed adjacent to the anode, which is a light-transmitting electrode, in order to lower the driving voltage and improve the light emission luminance.
  • the details of the hole injection layer are described in JP-A-9-45479, JP-A-9-260062, JP-A-8-288069, etc.
  • materials used for the hole injection layer include: , Porphyrin derivatives, phthalocyanine derivatives, oxazole derivatives, oxadiazole derivatives, triazole derivatives, imidazole derivatives, pyrazoline derivatives, pyrazolone derivatives, phenylenediamine derivatives, hydrazone derivatives, stilbene derivatives, polyarylalkane derivatives, triarylamine derivatives, carbazole derivatives, Indolocarbazole derivatives, isoindole derivatives, acene derivatives such as anthracene and naphthalene, fluorene derivatives, fluorenone derivatives, polyvinylcarbazole, aromatic amines introduced into the main chain or side chain Child material or oligomer, polysilane, a conductive polymer or oligomer
  • Examples of the triarylamine derivative include benzidine type represented by ⁇ -NPD (4,4′-bis [N- (1-naphthyl) -N-phenylamino] biphenyl), and MTDATA (4,4 ′, 4 ′′).
  • Examples include a starburst type represented by -tris [N- (3-methylphenyl) -N-phenylamino] triphenylamine), a compound having fluorene or anthracene in the triarylamine-linked core.
  • hexaazatriphenylene derivatives such as those described in JP-T-2003-519432 and JP-A-2006-135145 can also be used as a hole transport material.
  • the electron injection layer is a layer provided between the cathode and the light emitting layer in order to lower the driving voltage and improve the light emission luminance.
  • the cathode is composed of the light-transmitting electrode according to the present invention Is provided adjacent to the light-transmitting electrode, and “Organic EL element and its forefront of industrialization” (issued on November 30, 1998 by NTT)
  • the electrode material “(pages 123 to 166) is described in detail.
  • JP-A-6-325871, JP-A-9-17574, JP-A-10-74586, and the like Specific examples of materials preferably used for the electron injection layer are as follows. Metals represented by strontium and aluminum, alkali metal compounds represented by lithium fluoride, sodium fluoride, potassium fluoride, etc., alkali metal halide layers represented by magnesium fluoride, calcium fluoride, etc. Examples thereof include an alkaline earth metal compound layer typified by magnesium, a metal oxide typified by molybdenum oxide and aluminum oxide, and a metal complex typified by lithium 8-hydroxyquinolate (Liq).
  • Metals represented by strontium and aluminum alkali metal compounds represented by lithium fluoride, sodium fluoride, potassium fluoride, etc.
  • the electrode which has the light transmittance in this invention is a cathode
  • organic materials such as a metal complex
  • the electron injection layer is preferably a very thin film, and depending on the constituent material, the layer thickness is preferably in the range of 1 nm to 10 ⁇ m.
  • the hole transport layer is made of a hole transport material having a function of transporting holes.
  • the hole injection layer and the electron blocking layer also have the function of a hole transport layer.
  • the hole transport layer can be provided as a single layer or a plurality of layers.
  • the hole transport material has any of hole injection or transport and electron barrier properties, and may be either organic or inorganic.
  • triazole derivatives oxadiazole derivatives, imidazole derivatives, polyarylalkane derivatives, pyrazoline derivatives, pyrazolone derivatives, phenylenediamine derivatives, arylamine derivatives, amino-substituted chalcone derivatives, oxazole derivatives, styrylanthracene derivatives, fluorenone derivatives, hydrazone derivatives
  • Examples include stilbene derivatives, silazane derivatives, aniline copolymers, conductive polymer oligomers, and thiophene oligomers.
  • hole transport material those described above can be used, but porphyrin compounds, aromatic tertiary amine compounds and styrylamine compounds can be used, and in particular, aromatic tertiary amine compounds can be used. preferable.
  • aromatic tertiary amine compounds and styrylamine compounds include N, N, N ′, N′-tetraphenyl-4,4′-diaminophenyl, N, N′-diphenyl-N, N′— Bis (3-methylphenyl)-[1,1′-biphenyl] -4,4′-diamine (abbreviation: TPD), 2,2-bis (4-di-p-tolylaminophenyl) propane, 1,1 -Bis (4-di-p-tolylaminophenyl) cyclohexane, N, N, N ', N'-tetra-p-tolyl-4,4'-diaminobiphenyl, 1,1-bis (4-di-p -Tolylaminophenyl) -4-phenylcyclohexane, bis (4-dimethylamino-2-methylphenyl) phenylmethane, bis (4-di-p
  • the hole transport material may be formed by a known method such as a vacuum deposition method, a spin coating method, a casting method, a printing method including an ink jet method, and an LB method (Langmuir Brodget, Langmuir Brodgett method). Thus, it can be formed by thinning.
  • the layer thickness of the hole transport layer is not particularly limited, but is usually about 5 nm to 5 ⁇ m, preferably 5 to 200 nm.
  • the hole transport layer may have a single layer structure composed of one or more of the above materials.
  • the p property can be increased by doping impurities into the material of the hole transport layer.
  • Examples thereof include JP-A-4-297076, JP-A-2000-196140, 2001-102175 and J.P. Appl. Phys. 95, 5773 (2004), and the like.
  • the electron transport layer is made of a material having a function of transporting electrons, and in a broad sense, an electron injection layer and a hole blocking layer are also included in the electron transport layer.
  • the electron transport layer can be provided as a single layer structure or a stacked structure of a plurality of layers.
  • an electron transport material (also serving as a hole blocking material) constituting a layer portion adjacent to the light emitting layer is used as an electron transporting material. What is necessary is just to have the function to transmit.
  • any one of conventionally known compounds can be selected and used. Examples include nitro-substituted fluorene derivatives, diphenylquinone derivatives, thiopyran dioxide derivatives, carbodiimides, fluorenylidenemethane derivatives, anthraquinodimethane, anthrone derivatives, and oxadiazole derivatives.
  • a thiadiazole derivative in which the oxygen atom of the oxadiazole ring is substituted with a sulfur atom, and a quinoxaline derivative having a quinoxaline ring known as an electron-withdrawing group can also be used as a material for the electron transport layer. It can. Furthermore, a polymer material in which these materials are introduced into a polymer chain, or a polymer material having these materials as a polymer main chain can also be used.
  • metal complexes of 8-quinolinol derivatives such as tris (8-quinolinol) aluminum (abbreviation: Alq 3 ), tris (5,7-dichloro-8-quinolinol) aluminum, tris (5,7-dibromo-8- Quinolinol) aluminum, tris (2-methyl-8-quinolinol) aluminum, tris (5-methyl-8-quinolinol) aluminum, bis (8-quinolinol) zinc (abbreviation: Znq), etc. and the central metal of these metal complexes
  • a metal complex replaced with In, Mg, Cu, Ca, Sn, Ga, or Pb can also be used as a material for the electron transport layer.
  • the electron transport layer can be formed by thinning the above material by a known method such as a vacuum deposition method, a spin coating method, a casting method, a printing method including an inkjet method, and an LB method.
  • the thickness of the electron transport layer is not particularly limited, but is usually about 5 nm to 5 ⁇ m, preferably 5 to 200 nm.
  • the electron transport layer may have a single layer structure composed of one or more of the above materials.
  • blocking layer examples include a hole blocking layer and an electron blocking layer.
  • the blocking layer is a layer provided as necessary. For example, it is described in JP-A Nos. 11-204258 and 11-204359, and “Organic EL elements and the forefront of industrialization (published by NTT Corporation on November 30, 1998)” on page 237. Hole blocking (hole block) layer and the like.
  • the hole blocking layer has a function of an electron transport layer in a broad sense.
  • the hole blocking layer is made of a hole blocking material that has a function of transporting electrons but has a very small ability to transport holes, and recombines electrons and holes by blocking holes while transporting electrons. Probability can be improved.
  • the structure of an electron carrying layer can be used as a hole-blocking layer as needed.
  • the hole blocking layer is preferably provided adjacent to the light emitting layer.
  • the electron blocking layer has a function of a hole transport layer in a broad sense.
  • the electron blocking layer is made of a material that has the ability to transport holes and has a very small ability to transport electrons. By blocking holes while transporting holes, the probability of recombination of electrons and holes is improved. Can be made.
  • the structure of a positive hole transport layer can be used as an electron blocking layer as needed.
  • the layer thickness of the hole blocking layer applied to the present invention is preferably in the range of 3 to 100 nm, more preferably in the range of 5 to 30 nm.
  • the cathode constituted by dividing the separator according to the present invention is a light-transmitting electrode that functions to supply holes to the carrier transporting functional layer group and the light emitting layer, and is made of metal, alloy, organic or inorganic
  • conductive compounds or mixtures thereof include gold, aluminum, silver, magnesium, lithium, magnesium / copper mixtures, magnesium / silver mixtures, magnesium / aluminum mixtures, magnesium / indium mixtures, indium, lithium / aluminum mixtures, rare earth metals
  • oxide semiconductors such as ITO, ZnO, TiO 2, and SnO 2 can be used.
  • the semiconductor is composed of at least a thin-film metal or alloy, more preferably a nitrogen-containing compound.
  • An underlayer composed of Is preferably silver is configured to have an electrode layer is composed of the main component and the alloy.
  • suitable silver or an alloy containing silver as a main component as a light-transmitting cathode include the same materials as those described in the description of the anode. Alternatively, it may be made of an alloy containing silver (Ag). Examples of such alloys include silver / magnesium (Ag / Mg), silver / copper (Ag / Cu), silver / palladium (Ag / Pd), silver / palladium / copper (Ag / Pd / Cu), silver -Indium (Ag.In) etc. are mentioned.
  • the cathode can be produced by forming a thin film of these conductive materials by a method such as vapor deposition or sputtering.
  • the sheet resistance as the second electrode is several hundred ⁇ / sq.
  • the film thickness is usually selected from the range of 5 nm to 5 ⁇ m, preferably 5 to 200 nm.
  • the organic EL panel of the present invention has a structure divided into a plurality of light emitting areas (organic EL elements), and an anode constituting one of the divided light emitting areas constitutes the other adjacent light emitting area.
  • the structure is characterized in that it is electrically connected in series with the cathode.
  • FIG. 2 is a schematic cross-sectional view (Embodiment 1) showing an example of the configuration of the organic EL panel of the present invention having a plurality of organic EL elements.
  • a plurality of organic EL elements are arranged in a state of being separated from each other on a single transparent substrate (1) having a large area, An independent light emitting area is formed.
  • a plurality of organic EL elements composed of an anode (3), a separator (8), an organic functional layer unit (U), a cathode (7), etc. are arranged on the substrate (1).
  • the cathode (7) is formed in an electrically divided state between the two separators (8), and the cathode (7) constituting one of the divided light emitting areas is adjacent to the area indicated by the circular broken line portion.
  • the other light emitting area is configured to be electrically connected in series with the end of the anode (3) constituting the other light emitting area. By setting it as such a structure, a some organic EL element (OLED) can be connected in series.
  • the area from the left end of the cathode (7) in contact with the separator (8) to the right end of the anode (3) is the “light emitting area”, and is adjacent to the right end of the anode (3).
  • the other end of the cathode (7) in contact with the separator (8) of the other organic EL element (OLED) is the “non-light emitting area”.
  • FIG. 3 is a schematic sectional view (embodiment 2) showing an example having an insulating layer (12) in the configuration of the organic EL panel (P) of the present invention.
  • the basic configuration is the same as that of the first embodiment described with reference to FIG. 2, and an insulating layer (12) is provided between the anode (3) and the separator (8).
  • an insulating layer (12) is provided between the anode (3) and the separator (8).
  • the insulating layer is preferably formed so as to cover the end of the anode (3). Since the thickness of the organic functional layer unit (U) is reduced at the end of the anode, short-circuiting can be made difficult by forming an insulating layer.
  • the portion where the insulating layer is formed can be a non-light emitting region that does not contribute to light emission.
  • the insulating layer may be formed as long as the insulating layer is formed so that the anode is exposed in the light emitting area.
  • the size of the light emitting region is not particularly limited, and is appropriately set according to the use of the organic EL panel.
  • Examples of the material for forming the insulating layer include photo-curing resins such as photosensitive polyimide resins and acrylic resins, thermosetting resins, and inorganic materials.
  • a method for forming the insulating layer a general method such as a photolithography method or a printing method can be used, but it is particularly preferable to form the insulating layer by a photolithography method.
  • Embodiment 3 Forming a gas barrier layer on a substrate
  • the organic EL panel (P) shown in FIG. 4 is a schematic cross-sectional view (Embodiment 3) showing an example of a configuration having a gas barrier layer (2) on a substrate.
  • the basic configuration is the same as the configuration described in FIG. 3 of the second embodiment, except that a gas barrier layer (2) is formed between the base material (1) and the anode (3). .
  • a higher-order gas barrier property can be imparted to a flexible resin substrate having a higher water vapor permeability and the like as a substrate than a glass substrate.
  • ⁇ Gas barrier layer> By forming a gas permeable gas barrier layer (2) on at least one side or both sides of the substrate (1) on the side where the anode (3, first electrode) is formed, moisture, oxygen, etc. Intrusion of materials that cause deterioration of the constituent materials of the organic EL element can be suppressed.
  • the gas barrier layer (2) may be not only an inorganic material film but also a film made of a composite material with an organic material or a hybrid film obtained by laminating these films.
  • water vapor permeability measured by a method in accordance with JIS (Japanese Industrial Standard) -K7129 (2008) (environmental condition: 25 ⁇ 0.5 ° C., relative humidity: 90 ⁇ 2) %) Is about 0.01 g / m 2 ⁇ 24 h or less
  • the oxygen permeability measured by a method according to JIS-K7126 (2006) is about 0.01 ml / m 2 ⁇ 24 h ⁇ atm or less
  • the resistivity is It is preferably a light-transmitting insulating film having gas barrier properties such that 1 ⁇ 10 12 ⁇ ⁇ cm or more and light transmittance is about 80% or more in the visible light region.
  • any material for forming the gas barrier layer (2) can be used as long as it can suppress the intrusion of a gas such as water or oxygen into the organic EL element, which causes deterioration of the organic EL element. .
  • the gas barrier layer (2) is made of an inorganic material such as silicon oxide, silicon nitride, silicon oxynitride, silicon carbide, silicon oxycarbide, aluminum oxide, aluminum nitride, titanium oxide, zirconium oxide, niobium oxide, and molybdenum oxide. It can be comprised with a film, Preferably, it is the structure which uses silicon compounds, such as a silicon nitride and a silicon oxide, as a main raw material.
  • a conventionally known thin film forming method can be appropriately selected and used.
  • a vacuum deposition method, a sputtering method, a magnetron sputtering method, a molecular beam epitaxy method, a cluster ion beam method, an ion plate method can be used.
  • Coating method, plasma polymerization method, atmospheric pressure plasma polymerization method (see JP 2004-68143 A), plasma CVD (Chemical Vapor Deposition) method, laser CVD method, thermal CVD method, ALD (atomic layer deposition) method, A wet coating method using polysilazane or the like can also be applied.
  • Embodiment 4 Arrangement pattern of organic EL elements
  • the plurality of light-emitting areas have a pattern arranged in parallel in a stripe shape.
  • FIG. 5 is a top view and a schematic cross-sectional view (embodiment 4) showing an example of an organic EL panel in which a plurality of light emitting areas are arranged in a stripe shape.
  • FIG. 5A shows an example in which light emitting areas composed of strip-shaped organic EL elements (OLEDs) are arranged in stripes on a substrate (1) having a large area.
  • OLEDs organic EL elements
  • FIG. 5A n organic EL elements (OLEDs) from OLED 1 to OLED n are arranged in parallel.
  • the number of OLEDs to be arranged cannot be unconditionally defined by the size of the substrate or the size of the OLEDs, but the minimum configuration uses two OLEDs.
  • it is preferably in the range of 2 to 20, more preferably in the range of 2 to 10.
  • the size of the light emitting area by OLED is 0.5 cm wide ⁇ 10 cm long ⁇ 5 cm wide ⁇ 10 cm long, preferably Is within the range of width 1.0 cm ⁇ length 10 cm to width 5 cm ⁇ length 10 cm.
  • the area of the light emitting area can be appropriately selected depending on the size of the substrate and the number of OLEDs arranged.
  • the width of the “non-light emitting area” shown in FIG. 5 is preferably within a range of about 0.2 to 1.0 mm.
  • FIG. 5B is a schematic cross-sectional view of the organic EL panel (P) having the configuration shown in FIG. 5A, in which n OLEDs from OLED 1 to OLED n are arranged in parallel.
  • the end of the anode (3) constituting one divided light emitting area and the end of the cathode (7) constituting the other adjacent light emitting area are electrically connected in series. It is connected to the.
  • the anode (3) of the OLED disposed at one end for example, the leftmost OLED 1 shown in FIG. 5B
  • the OLED disposed at the other end for example, FIG. 5 (b)
  • the cathode (7) of OLED n at the right end is connected by a wiring (18), and an applied power source (13) is provided in the circuit so that each OLED emits light. Power supply.
  • FIG. 6A shows a circuit diagram of a conventional organic EL panel
  • FIG. 6B shows a circuit diagram of the organic EL panel of the present invention.
  • FIG. 6A is a circuit diagram of a conventional organic EL panel (P), and is a circuit diagram when configured with a single large organic EL element (OLED).
  • a voltage V and a current I are applied to cause light emission.
  • a large-capacity current I flows through a large area OLED. Occur, and uneven brightness tends to occur. Since the luminance of the organic EL element becomes higher as the flowing current increases, the occurrence of such a current difference tends to cause uneven luminance.
  • the voltage N is applied to the organic EL element from the applied power supply (13).
  • ⁇ V current I is applied to cause light emission, but the current flowing through each organic EL element (OLED) is I / N, and it is difficult for current differences between the organic EL elements to occur, so luminance unevenness is unlikely to occur. Therefore, it is possible to realize a large-sized organic EL panel having excellent light emission uniformity.
  • FIG. 7 is a schematic sectional drawing (embodiment 5) which shows an example of the structure which provided the sealing member by the structure of the organic electroluminescent panel of this invention.
  • the organic EL panel (P) shown in FIG. 7 the organic EL panel (P) having a plurality of organic EL elements (OLED) formed up to the cathode shown in FIG. An example of forming a member is shown.
  • the sealing member may be disposed so as to cover the display area of the organic EL element, and may be concave or flat. Moreover, if it has transparency, electrical insulation will not be specifically limited.
  • a light transmissive glass substrate a resin substrate, a film, a metal film (metal foil) having flexibility, and the like
  • the glass substrate include soda-lime glass, barium / strontium-containing glass, lead glass, aluminosilicate glass, borosilicate glass, barium borosilicate glass, and quartz.
  • the resin substrate include polycarbonate, acrylic, polyethylene terephthalate, polyether sulfide, and polysulfone.
  • sealing adhesive polyurethane-based, polyester-based, epoxy-based, acrylic-based adhesives can be used. You may use a hardening
  • a hot melt lamination method, an extrusion lamination method and a coextrusion lamination method can also be used, but a dry lamination method is preferred.
  • the sealing member a resin substrate and a crow substrate can be preferably used from the viewpoint of reducing the thickness of the organic EL element.
  • the resin substrate has a water vapor transmission rate of 1 ⁇ 10 ⁇ 3 g / m 2 .multidot.m at a temperature of 25 ⁇ 0.5 ° C. and a relative humidity of 90 ⁇ 2% RH measured by a method according to JIS K 7129-1992.
  • the oxygen permeability measured by a method according to JIS K 7126-1987 is preferably 1 ⁇ 10 ⁇ 3 ml / m 2 ⁇ 24 h ⁇ atm (1 atm is 1.01325 ⁇ 10 5 a Pa) equal to or lower than a temperature of 25 ⁇ 0.5 ° C.
  • water vapor permeability at a relative humidity of 90 ⁇ 2% RH is preferably not more than 1 ⁇ 10 -3 g / m 2 ⁇ 24h.
  • an inert gas such as nitrogen or argon, or an inert liquid such as fluorocarbon or silicon oil is injected in the gas phase and liquid phase.
  • an inert gas such as nitrogen or argon, or an inert liquid such as fluorocarbon or silicon oil is injected in the gas phase and liquid phase.
  • the gap between the sealing member and the display area of the organic EL element can be evacuated, or a hygroscopic compound can be sealed in the gap.
  • the method for producing an organic E panel of the present invention is a method for producing an organic EL panel having an organic electroluminescence element having a light transmittance of 50% or more at a wavelength of 550 nm when not emitting light having the above-described configuration,
  • a light emitting area composed of at least an anode, an organic functional layer unit, and a cathode is formed on a substrate by dividing into a plurality of parts, and the cathode is separated by a separator provided on the anode.
  • a pattern is formed, and the anode constituting one of the divided light emitting areas is electrically connected in series with the cathode constituting the other neighboring light emitting area, and the anode, cathode and separator are connected to the photo It is formed by a lithography method.
  • a manufacturing method in which an insulating layer is formed between the anode and the separator using a photolithography method is a preferred embodiment.
  • a gas barrier layer (2) is formed on the substrate (1) by vacuum deposition, sputtering, CVD, or wet coating.
  • the anode (3), the insulating layer (12), and the separator (8) are formed by photolithography, the organic functional layer unit (U) and the cathode (7) are formed by vapor deposition, and finally wet.
  • the sealing adhesive (9) by a coating method or the like, the entire surface is sealed with a sealing substrate (11) having a gas barrier layer (10) to produce an organic EL panel (P). .
  • the anode (3), the insulating layer (12), and the separator (8) having a desired pattern can be formed by etching (patterning) using a photolithography method.
  • etching patterning
  • a photolithography method By applying a photolithography method to the above formation, a highly accurate and fine anode (3), insulating layer (12), and separator (8) can be formed, and an extremely narrow non-light emitting area can be formed.
  • the photolithographic method applicable to the present invention includes resist coating, (preheating), exposure, development, rinsing, (pretreatment), etching, and resist stripping, and then the anode (3), the insulating layer.
  • This is a method for forming (12) and the separator (8) with a desired high-definition pattern.
  • a conventionally known general photolithography method can be used as appropriate.
  • a positive type resist or a negative type resist can be used.
  • preheating or prebaking can be performed as necessary.
  • a pattern mask having a desired pattern may be disposed, and light having a wavelength suitable for the resist used, generally ultraviolet light may be irradiated thereon.
  • development can be performed with a developer that is compatible with the resist used.
  • the resist pattern is formed by stopping the development with a rinse solution such as water and washing.
  • the formed resist pattern can be engraved by etching after pre-processing or post-baking as necessary. After etching, the remaining resist is peeled off to obtain an anode (3), an insulating layer (12), and a separator (8) having a desired pattern.
  • the photolithography method applied to the present invention is a method generally recognized by those skilled in the art, and a specific application mode can be easily selected according to the purpose by those skilled in the art. it can.
  • FIG. 8 is a process flow diagram (Embodiment 6) showing an example of the manufacturing procedure of the organic EL panel (P) of Embodiment 5 shown in FIG.
  • a gas barrier layer (2) is formed on a light-transmitting substrate (1).
  • the gas barrier layer (2) can be formed by vacuum deposition, sputtering, magnetron sputtering, molecular beam epitaxy, cluster ion beam, ion plating, plasma polymerization, atmospheric pressure plasma It is formed by a wet coating method using a combination method, a plasma CVD method, polysilazane, or the like.
  • a plurality of light-transmitting anodes (3) are separated from each other at predetermined positions on the gas barrier layer (2) by using a photolithography method. Form.
  • an insulating layer (12) is formed in a specific area (edge) on the anode by the same photolithography method.
  • a separator (8) is formed on the formed insulating layer (12) using the same photolithography method.
  • the carrier transport function layer group 1 (4, for example, a hole injection layer and a hole transport layer), the light emitting layer (5), the carrier transport function layer group 2 A plurality of organic functional layer units (U) composed of (6, electron transport layer, etc.) are formed.
  • Each of the organic functional layer units can be formed by spin coating, casting, ink jet, vapor deposition, printing, etc., but it is easy to obtain a homogeneous layer and is formed with high accuracy. It is preferable to apply a vapor deposition method using a fine mask (M) in that it can be performed. Specifically, each raw material for forming each organic functional layer unit is filled in a heating boat for vapor deposition, the heating boat is heated, and on the anode (3) having light transmittance through a fine mask, A pattern of each layer of the organic functional layer unit (U) is formed.
  • M fine mask
  • a different forming method may be applied to each layer constituting the organic functional layer unit layer (U).
  • the vapor deposition conditions vary depending on the type of compound used, but generally the boat heating temperature is in the range of 50 to 450 ° C., and the degree of vacuum is 1 ⁇ 10 ⁇ 6 to 1 ⁇ .
  • Each condition is preferably selected as appropriate within the range of 10 ⁇ 2 Pa, the deposition rate of 0.01 to 50 nm / second, the substrate temperature of ⁇ 50 to 300 ° C., and the layer thickness of 0.1 to 5 ⁇ m. .
  • a light-transmitting cathode (7) is formed on the entire surface of a specific area separated by two separators (8) on the plurality of organic functional layer units (U). ). At this time, it is formed so as to be electrically connected to the end portion of the anode (3) of one organic EL element formed at an adjacent position via a conductive adhesive or the like.
  • a cathode forming raw material is filled in a vapor deposition heating boat, the heating boat is heated, and the organic functional layer unit (U) and the adjacent anode (3) are passed through a fine mask.
  • a cathode (7) is formed. At this time, the cathode (7) and the adjacent anode (3) are electrically connected by a conductive adhesive (not shown).
  • a light-transmitting cathode is an underlayer composed of a nitrogen-containing compound, and a thin-film silver layer composed of silver or an alloy containing silver as a main component on the underlayer (
  • One of the preferred embodiments is a structure having a cathode.
  • FIG. 9 shows a structure in which a base layer (14) and a thin film silver layer (15) made of silver or an alloy containing silver as a main component are provided thereon as a cathode.
  • the silver atom is first a compound having a nitrogen atom, and more specifically, on the surface of the underlayer containing an asymmetric compound having a nitrogen atom having an unshared electron pair that does not participate in aromaticity having an affinity for the silver atom.
  • the film is formed by single-layer growth type (Frank-van der Merwe: FM type) film formation in which a two-dimensional nucleus is formed at the center and a two-dimensional single crystal layer is formed around the two-dimensional nucleus.
  • a thin silver film with high homogeneity can be formed.
  • the material constituting the underlayer is not particularly limited, and can suppress aggregation of silver, which is a constituent material of the cathode formed thereon, and includes compounds containing nitrogen atoms.
  • the nitrogen atom-containing compound that can be used to form the underlayer (14) is not particularly limited as long as it is a compound containing a nitrogen atom in the molecule, but a heterocycle having a nitrogen atom as a heteroatom. A compound having is preferred.
  • heterocycle having a nitrogen atom as a hetero atom examples include aziridine, azirine, azetidine, azeto, azolidine, azole, azinane, pyridine, azepan, azepine, imidazole, pyrazole, oxazole, thiazole, imidazoline, pyrazine, morpholine, thiazine, indole, Examples include isoindole, benzimidazole, purine, quinoline, isoquinoline, quinoxaline, cinnoline, pteridine, acridine, carbazole, benzo-C-cinnoline, porphyrin, chlorin and choline.
  • the nitrogen atom-containing compound contained in the underlayer (14) is preferably an aromatic heterocyclic compound having a nitrogen atom having an unshared electron pair not involved in aromaticity.
  • nitrogen atom-containing compounds include Exemplified Compound Nos. Described in paragraphs (0097) to (0221) of JP-A-2015-046364. 1-No. 134.
  • FIG. 10 is an example of a configuration of an organic EL element applicable to the present invention, and schematically shows a configuration in which an optical adjustment layer (16) is formed on the thin film silver layer (15) having the configuration described in FIG. It is sectional drawing (Embodiment 6).
  • the optical adjustment layer applicable to the present invention means a layer that plays a role of improving the transmittance of the light transmissive material by the optical interference action.
  • an existing compound can be used without particular limitation as long as an appropriate refractive index is obtained.
  • a compound to which a vacuum deposition method can be applied is preferable from the viewpoint that a film can be formed on the organic EL cathode without damage.
  • Al 2 O 3 reffractive index 1.6
  • CeO 3 reffractive index 2.2
  • Ga 2 O 3 reffractive index 1.5
  • HfO 2 reffractive index
  • ITO indium tin oxide, refractive index 2.1
  • IZO indium zinc oxide, refractive index 2.1
  • MgO indium zinc oxide, refractive index 2.1
  • MgO indium zinc oxide, refractive index 2.1
  • MgO reffractive index 1.7
  • Nb 2 O 5 reffractive index
  • SiO 2 reffractive index 1.5
  • Ta 2 O 5 reffractive index 2.2
  • TiO 2 refractive index 2.3 to 2.5
  • Y 2 O 3 reffractive index 1.
  • connection part of an organic electroluminescent panel and an external electrode is the structure electrically connected by the electroconductive adhesive, and also the external electrode is a flexible printed circuit (with light transmittance) ( FPC) is a preferred form.
  • FIG. 11 is a schematic diagram showing an example of an electrical connection method between an organic EL panel and external electrodes applicable to the present invention.
  • FIG. 11 a flexible printed circuit having optical transparency as an external electrode with respect to the extraction electrode (17) provided at both ends of the organic EL panel (P) in which a plurality of organic EL elements (OLED) are arranged in parallel.
  • FPC Flexible printed circuit
  • a thin and soft base film polyimide, etc.
  • FPC which is an electrical connection unit has a circuit part on the front side of the flexible substrate and wiring on the back side.
  • the flexible substrate constituting the electrical connection unit (FPC) is not particularly limited as long as it is a transparent and flexible plastic material having sufficient mechanical strength.
  • Polyimide resin (PI), polycarbonate resin, Polyethylene terephthalate resin (PET), polyethylene naphthalate resin (PEN), cycloolefin resin (COP) and the like can be mentioned, and polyimide resin (PI), polyethylene terephthalate resin (PET), polyethylene naphthalate resin (PEN) are preferable. Is preferred.
  • the circuit part on the front surface and the wiring on the back surface are preferably made of a conductive metal material, and examples thereof include gold, silver, copper, and ITO.
  • the wiring is formed of copper. It is preferable.
  • the conductive adhesive for electrically connecting the transparent FPC and the organic EL panel is not particularly limited as long as it is a member having conductivity, but an anisotropic conductive film (ACF), conductive paste, or metal paste. It is a preferred embodiment.
  • anisotropic conductive film examples include a layer having fine conductive particles having conductivity mixed with a thermosetting resin.
  • the conductive particle-containing layer that can be used in the present invention is not particularly limited as long as it is a layer containing conductive particles as an anisotropic conductive member, and can be appropriately selected according to the purpose.
  • Examples of the conductive particles that can be used as the anisotropic conductive member according to the present invention include metal particles and metal-coated resin particles.
  • commercially available ACFs include low-temperature curing ACFs that can also be applied to resin films, such as MF-331 (manufactured by Hitachi Chemical).
  • the metal particles include nickel, cobalt, silver, copper, gold, and palladium. These may be used individually by 1 type and may use 2 or more types together. Among these, nickel, silver, and copper are preferable. In order to prevent these surface oxidations, particles having gold or palladium on the surface may be used. Furthermore, you may use what gave the metal film and the insulating film with the organic substance on the surface.
  • metal-coated resin particles examples include particles in which the surface of the resin core is coated with any metal of nickel, copper, gold, and palladium. Similarly, particles obtained by applying gold or palladium to the outermost surface of the resin core may be used. Further, a resin core whose surface is coated with a metal protrusion or an organic material may be used.
  • a commercially available metal nanoparticle paste such as a silver particle paste, a silver-palladium particle paste, a gold particle paste, a copper particle paste, or the like, can be appropriately selected and used.
  • the metal paste include silver pastes for organic EL element substrates (CA-6178, CA-6178B, CA-2500E, CA-2503-4, CA-2503N, CA-271, etc., sold by Daiken Chemical Co., Ltd.
  • the organic electroluminescence panel of the present invention achieves luminance uniformity and can be suitably used for various smart devices such as surface light emitters of various lighting devices and smartphones and tablets.

Abstract

The present invention addresses the issue of providing: an organic EL panel comprising light-transmissive organic EL elements, having a wide light-emitting area comprising a plurality of divided light-emission areas, and having improved luminance uniformity and stability; and a production method therefor. This organic EL panel has organic EL elements having a light-transmittance of at least 50% at a wavelength of 550 nm during non-emission of light. The organic EL elements are characterized by: the light-emission areas, comprising at least a positive electrode, an organic functional layer unit, and a negative electrode, being divided into a plurality of areas upon a substrate; the positive electrodes and the negative electrodes constituting the light-emission areas each comprising light-transmissive electrodes; the negative electrodes being divided by separators provided upon the positive electrodes; and a positive electrode constituting one of the divided light-emission areas being electrically connected in series to a negative electrode constituting another adjacent light-emission area.

Description

有機エレクトロルミネッセンスパネル及びその製造方法Organic electroluminescence panel and manufacturing method thereof
　本発明は、各種表示装置（以下、「ディスプレイ」ともいう。）及び照明装置等に適用される光透過性を有する有機エレクトロルミネッセンスパネルとその製造方法に関し、更に詳しくは、本発明は、光透過性を有する有機エレクトロルミネッセンス素子より構成される発光エリアを複数個配置し、広い発光面積で、輝度均一性及び安定性が向上した有機エレクトロルミネッセンスパネルとその製造方法に関する。 The present invention relates to a light-transmitting organic electroluminescence panel applied to various display devices (hereinafter, also referred to as “displays”), lighting devices, and the like, and more specifically, the present invention relates to light transmission. TECHNICAL FIELD The present invention relates to an organic electroluminescence panel in which a plurality of light emitting areas composed of organic electroluminescence elements having a property are arranged, a wide light emitting area, and brightness uniformity and stability are improved, and a method for manufacturing the same.
　有機材料のエレクトロルミネッセンス（ｅｌｅｃｔｒｏ　ｌｕｍｉｎｅｓｃｅｎｃｅ：以下、「ＥＬ」と略記する。）を利用した有機エレクトロルミネッセンスＬ素子（以下、「有機ＥＬ素子」と略記する。）は、数Ｖ～数十Ｖ程度の低電圧で発光が可能な薄膜型の完全固体素子であり、高輝度、高発光効率、薄型、軽量といった多くの優れた特徴を有する。このため、有機ＥＬ素子は、各種ディスプレイのバックライト、スマートデバイス、照明光源等の面発光体として近年注目されている。 An organic electroluminescence L element (hereinafter abbreviated as “organic EL element”) using an organic material electroluminescence (hereinafter abbreviated as “EL”) has a voltage of about several V to several tens of volts. It is a thin-film, completely solid element that can emit light at a low voltage, and has many excellent features such as high brightness, high luminous efficiency, thinness, and light weight. For this reason, organic EL elements have attracted attention in recent years as surface light emitters such as backlights for various displays, smart devices, and illumination light sources.
　このような有機ＥＬ素子は、２枚の対向する電極間に有機材料からなる発光層を挟持させた構成であり、発光層で生じた発光光は電極を透過して外部に取り出される。このため、２枚の電極のうちの少なくとも一方は光透過性を有する電極（以下、透明電極ともいう。）として構成される。 Such an organic EL element has a structure in which a light emitting layer made of an organic material is sandwiched between two opposing electrodes, and light emitted from the light emitting layer is transmitted through the electrode and taken out to the outside. For this reason, at least one of the two electrodes is configured as a light-transmitting electrode (hereinafter also referred to as a transparent electrode).
　光透過性を有する電極としては、酸化インジウム・スズ（ＳｎＯ２－Ｉｎ２Ｏ３：Ｉｎｄｉｕｍ　Ｔｉｎ　Ｏｘｉｄｅ、以下、「ＩＴＯ」と略記する。）等の酸化物半導体系の材料が一般的に用いられている。 As an electrode having optical transparency, an oxide semiconductor material such as indium tin oxide (SnO 2 —In 2 O 3 : Indium Tin Oxide, hereinafter abbreviated as “ITO”) is generally used. ing.
　また、有機エレクトロルミネッセンス素子を用いたディスプレイにおいて、その適用分野を拡大させる観点より、両面発光型の光透過性を有する有機エレクトロルミネッセンス素子の検討が、例えば、特表２００８－５２４８１９号公報、特開２０１３－００４２４５号公報、特開２０１３－２４２９９８号公報等で開示されている。 In addition, in a display using an organic electroluminescence element, from the viewpoint of expanding its application field, studies on an organic electroluminescence element having a double-sided light-transmitting property are disclosed in, for example, JP-T-2008-524819, JP, JP-A-2013-004245, JP-A-2013-242998, and the like.
　このような両面発光型の有機エレクトロルミネッセンス素子においては、発光層を挟んで、陽極及び陰極の両極が光透過性を有する透明電極対で構成されており、このような光透過性を有する電極としては、前述のとおりＩＴＯを用いることが一般的であったが、ＩＴＯは仕事関数が大きいため、陽極としての性能には優れるが、陰極としての性能が劣る傾向にあった。このため、両面に光透過性を有する電極を用いる光透過性を有するディスプレイ用の電極としては、現状技術で高い性能を得るためには、陽極、陰極共にＩＴＯ－ＩＴＯの電極を用いるのではなく、陽極ＩＴＯ－陰極アルミニウム等の電極を用い、陰極の面積をできるだけ小さくすることで発光部とシースルー部分（光透過部）を設ける光透過性を有するディスプレイが開示されている（例えば、特許文献１参照。）。また、陰極として電気伝導率の高い銀や銀とアルミニウムの合金を用いて構成された光透過性を有する電極が知られているが、光透過性の有機エレクトロルミネッセンス素子においては、陽極及び陰極に用いる薄膜金属層や酸化物半導体の多くは、抵抗値が高く、電圧降下が大きく、特に、発光効率を向上させるために、光透過性を有する電極を薄膜化した場合や、素子の発光面積を大面積化した場合にはシート抵抗値が大きくなり、輝度均一性が大きく低下するという問題を抱えており、将来の大面積化や高輝度化を目指した有機エレクトロルミネッセンス素子の開発に対し大きな障害になっている。 In such a double-sided light emitting organic electroluminescent element, both the anode and the cathode are composed of a transparent electrode pair having light transmittance across the light emitting layer, and as such a light transmitting electrode, As described above, ITO was generally used. However, since ITO has a large work function, the performance as an anode was excellent, but the performance as a cathode tended to be inferior. For this reason, as a display electrode having a light transmitting property using electrodes having a light transmitting property on both sides, in order to obtain high performance with the current technology, both the anode and the cathode are not ITO-ITO electrodes. In addition, there is disclosed a light-transmitting display in which an electrode such as anode ITO-cathode aluminum is used and a light-emitting portion and a see-through portion (light transmission portion) are provided by minimizing the area of the cathode (for example, Patent Document 1). reference.). Further, a light-transmitting electrode composed of silver having a high electrical conductivity or an alloy of silver and aluminum is known as a cathode. However, in a light-transmitting organic electroluminescence element, the anode and the cathode Many of the thin film metal layers and oxide semiconductors used have a high resistance value and a large voltage drop.In particular, in order to improve the light emission efficiency, the light-transmitting electrode is made thin, or the light emitting area of the element is reduced. If the area is increased, the sheet resistance value will increase and the luminance uniformity will be greatly reduced. This will be a major obstacle to the development of organic electroluminescence devices that aim to increase the area and brightness in the future. It has become.
　有機エレクトロルミネッセンス素子の大型化により、発光層の各位置において、電流密度を面方向で均一化することが困難となり、その結果、輝度ムラ、素子寿命差あるいは色度ムラが生じる要因としては、以下のような現象が推測される。 Due to the increase in size of the organic electroluminescence device, it is difficult to make the current density uniform in the plane direction at each position of the light emitting layer, and as a result, the following causes of brightness unevenness, device life difference or chromaticity unevenness are as follows: Such a phenomenon is presumed.
　大面積化に伴う輝度ムラの発生要因としては、発光画面を大型化することで、画面内で電流が多く流れる箇所と少なくしか流れない箇所とが存在するため、有機ＥＬ素子全体として輝度ムラが生じる。有機ＥＬ素子の輝度は、流れる電流が大きくなるほど高くなるため、電流が多く流れる箇所と少なくしか流れない箇所が存在すると両者の間で輝度の差が生じ、輝度ムラ発生の要因となる。 The cause of uneven brightness due to the increase in area is that by increasing the size of the light emitting screen, there are places where a large amount of current flows and places where only a small amount of current flows in the screen. Arise. Since the luminance of the organic EL element increases as the flowing current increases, the presence of a portion where a large amount of current flows and a portion where a small amount of current flows causes a difference in luminance between the two, which causes luminance unevenness.
　また、大型化に伴い有機ＥＬ素子内のそれぞれの発光領域において寿命差が発生する。これは、電流が多く流れる箇所と少なくしか流れない箇所とで、有機ＥＬ素子の寿命が変わってしまう。一般に、流れる電流の多い部分は寿命が短くなる。このため、電流が均一に流れる素子と比べると、寿命の短い箇所が存在してしまい、有機ＥＬ素子としての寿命が短くなってしまう。 Moreover, a life difference occurs in each light emitting region in the organic EL element as the size increases. This is because the lifetime of the organic EL element is changed between a portion where a large amount of current flows and a portion where a small amount of current flows. In general, the life of a portion where a large amount of current flows is shortened. For this reason, as compared with an element in which current flows uniformly, a portion having a short lifetime exists, and the lifetime as an organic EL element is shortened.
　このような問題を解決するために、従来、種々の技術が提案されてきた。 In order to solve such problems, various techniques have been conventionally proposed.
　例えば、電圧印加用の取出部（上記端子部）を多数箇所設ける技術が、特開平５－３１５０７３号公報にて開示されている。しかし、有機ＥＬ素子が組み込まれる携帯端末等の装置は大きさが限定されるため、有機ＥＬ素子の大きさも限定される。すなわち、有機ＥＬ素子の発光面積を大きくするためには、端子部の総面積を小さくしなければならない。また、端子部と外部駆動回路とを接続する配線が占める領域の割合も考慮しなければならない。したがって、この従来技術のように取出部を多数設けることは、上記問題を解決するには有効であるが、実用上採用することは極めて困難である。 For example, Japanese Patent Laid-Open No. 5-315073 discloses a technique of providing a plurality of voltage application extraction portions (the terminal portions). However, since the size of a device such as a portable terminal in which the organic EL element is incorporated is limited, the size of the organic EL element is also limited. That is, in order to increase the light emitting area of the organic EL element, the total area of the terminal portion must be reduced. In addition, it is necessary to consider the ratio of the area occupied by the wiring connecting the terminal portion and the external drive circuit. Therefore, it is effective to solve the above problems by providing a large number of extraction portions as in this prior art, but it is extremely difficult to adopt in practice.
　一方、発光領域を複数に分割し、各発光領域を直列で接続するライン配置方式の光源に関する技術も提案されている（例えば、特許文献２を参照。）。より具体的には、複数の薄型発光素子（発光領域）を直列に接続し、さらに各薄型発光素子の面積を等しくすることで、各々の発光素子における電流密度を等しくし、これにより各薄型発光素子の輝度を等しくする技術である。また、複数の発光領域を設け、物理的に隣接する発光領域の光透過性を有する電極間に絶縁部を設け、複数の発光領域が電気的に直列に接続された構成の有機ＥＬ素子が開示されている（例えば、特許文献３参照。）。 On the other hand, a technique relating to a light source of a line arrangement method in which a light emitting area is divided into a plurality of parts and the light emitting areas are connected in series has also been proposed (see, for example, Patent Document 2). More specifically, a plurality of thin light emitting elements (light emitting regions) are connected in series, and the area of each thin light emitting element is made equal, so that the current density in each light emitting element is made equal, thereby reducing each thin light emitting element. This is a technique for equalizing the brightness of elements. Also disclosed is an organic EL device having a structure in which a plurality of light emitting regions are provided, an insulating portion is provided between light-transmitting electrodes of physically adjacent light emitting regions, and the plurality of light emitting regions are electrically connected in series. (For example, see Patent Document 3).
　しかしながら、上記特許文献２及び特許文献３に開示された実施例等に基づいて有機ＥＬ素子を作製しても、各発光領域における陽極と陰極とが短絡してしまったり、光らない発光領域が生じてしまったりするという、不良が生じやすいと言う問題が生じることがあった。 However, even when an organic EL element is manufactured based on the examples disclosed in Patent Document 2 and Patent Document 3, the anode and the cathode in each light-emitting region are short-circuited, or a light-emitting region that does not emit light is generated. There was a problem that it was easy to cause defects.
　一方、透明基板上に、第１透明電極、絶縁性の隔壁、有機ＥＬ層と、当該隔壁に分断されている第２透明電極から構成される透明有機ＥＬ素子が開示されている（例えば、特許文献４参照。）。 On the other hand, a transparent organic EL element comprising a first transparent electrode, an insulating partition, an organic EL layer and a second transparent electrode divided by the partition on a transparent substrate is disclosed (for example, a patent) Reference 4).
　特許文献４によれば、アライメントがずれても短絡を起こすことがなく第２透明電極層の抵抗を低減することができるとされている。しかしながら、特許文献４で開示されている具体的な構成について検討を進めた結果、分割されている各発光エリアを構成している第１透明電極と第２透明電極とが直接接続さている構成ではないため、各有機ＥＬ素子における電流値が高くなり、発光の不均一性を生じ、かつ過酷な条件で使用された場合には、各電極を接続している配線の切断や電極間での短絡を起こしやすいことが判明した。 According to Patent Document 4, the resistance of the second transparent electrode layer can be reduced without causing a short circuit even if the alignment is shifted. However, as a result of studying the specific configuration disclosed in Patent Document 4, as a result of the configuration in which the first transparent electrode and the second transparent electrode constituting each divided light emitting area are directly connected, Therefore, the current value in each organic EL element becomes high, causing non-uniformity of light emission, and when used under harsh conditions, cutting the wiring connecting each electrode or short-circuiting between the electrodes It turned out to be easy to cause.
特開２０１２－０１４８５９号公報JP 2012-014859 A 特開２０００－１７３７７１号公報JP 2000-173771 A 特開２００５－１１６１９３号公報JP 2005-116193 A 特開２０１１－２１６３１７号公報JP 2011-216317 A
　本発明は、上記問題に鑑みてなされたものであり、その解決課題は、光透過性を有する有機エレクトロルミネッセンス素子より構成され、複数の分割された発光エリアより構成される広い発光面積を有し、輝度均一性及び安定性が向上した有機エレクトロルミネッセンスパネル及びその製造方法を提供することである。 The present invention has been made in view of the above problems, and a solution to the problem is a wide light-emitting area that is composed of a light-transmitting organic electroluminescence element and is composed of a plurality of divided light-emitting areas. Another object of the present invention is to provide an organic electroluminescence panel having improved luminance uniformity and stability and a method for manufacturing the same.
　本発明者は、上記課題に鑑み鋭意検討を進めた結果、両面発光型の光透過性を有する有機エレクトロルミネッセンス素子を具備し、当該有機エレクトロルミネッセンス素子は、基材上に、少なくとも光透過性を有する陽極、有機機能層ユニット及び光透過性を有する陰極より構成される発光エリアが、複数に分割され、当該陰極が前記陽極上に設けたセパレーターにより分離した構成であり、かつ、一方の発光エリアを構成する陽極が、他方の発光エリアを構成する陰極と、直列に電気的に接続されていることを特徴とする有機エレクトロルミネッセンスパネルにより、大発光面積化を可能とし、各有機ＥＬ素子における発光に必要な電流値を低減でき、輝度均一性及び安定性が向上した有機エレクトロルミネッセンスパネルを実現することができることを見出し、本発明に至った。 As a result of intensive studies in view of the above problems, the present inventor has an organic electroluminescent element having a double-sided light-transmitting property, and the organic electroluminescent element has at least a light transmitting property on a substrate. A light emitting area composed of an anode having an organic functional layer unit and a light-transmitting cathode is divided into a plurality of parts, and the cathode is separated by a separator provided on the anode, and one light emitting area The organic electroluminescence panel is characterized in that the anode constituting the light-emitting element is electrically connected in series with the cathode constituting the other light-emitting area. An organic electroluminescence panel with improved brightness uniformity and stability can be realized. Found that it is, it has led to the present invention.
　すなわち、本発明の上記課題は、下記の手段により解決される。 That is, the above-mentioned problem of the present invention is solved by the following means.
　１．非発光時の波長５５０ｎｍにおける光透過率が５０％以上である有機エレクトロルミネッセンス素子を有する有機エレクトロルミネッセンスパネルであって、
　前記有機エレクトロルミネッセンス素子は、基材上に、少なくとも陽極、有機機能層ユニット及び陰極より構成される発光エリアが、複数に分割されており、
　前記発光エリアを構成する前記陽極及び前記陰極が、いずれも光透過性を有する電極で構成され、
　前記陰極が、前記陽極上に設けたセパレーターにより分離した構成であり、
　かつ、分割されている一方の発光エリアを構成する陽極が、隣接する他方の発光エリアを構成する陰極と、直列に電気的に接続されていることを特徴とする有機エレクトロルミネッセンスパネル。 1. An organic electroluminescence panel having an organic electroluminescence element having a light transmittance of 50% or more at a wavelength of 550 nm when not emitting light,
In the organic electroluminescence element, a light emitting area composed of at least an anode, an organic functional layer unit, and a cathode is divided into a plurality of parts on a base material,
The anode and the cathode constituting the light emitting area are both composed of electrodes having light transmittance,
The cathode is separated by a separator provided on the anode,
An organic electroluminescence panel, wherein an anode constituting one of the divided light emitting areas is electrically connected in series with a cathode constituting the other adjacent light emitting area.
　２．前記陽極と前記セパレーターとの間に、絶縁層を有することを特徴とする第１項に記載の有機エレクトロルミネッセンスパネル。 2. 2. The organic electroluminescence panel according to claim 1, further comprising an insulating layer between the anode and the separator.
　３．前記基材が、光透過性を有するガラス基材又はフレキシブル性樹脂基材であることを特徴とする第１項又は第２項に記載の有機エレクトロルミネッセンスパネル。 3. The organic electroluminescence panel according to item 1 or 2, wherein the substrate is a glass substrate or a flexible resin substrate having optical transparency.
　４．前記フレキシブル性樹脂基材が、ガスバリアー層を有していることを特徴とする第３項に記載の有機エレクトロルミネッセンスパネル。 4. 4. The organic electroluminescence panel according to item 3, wherein the flexible resin substrate has a gas barrier layer.
　５．前記光透過性を有する陽極が、酸化物半導体又は薄膜の金属若しくは合金で構成されていることを特徴とする第１項から第４項までのいずれか一項に記載の有機エレクトロルミネッセンスパネル。 5. The organic electroluminescence panel according to any one of items 1 to 4, wherein the light-transmitting anode is made of an oxide semiconductor or a thin-film metal or alloy.
　６．前記光透過性を有する陰極が、少なくとも薄膜の金属又は合金で構成されていることを特徴とする第１項から第５項までのいずれか一項に記載の有機エレクトロルミネッセンスパネル。 6. The organic electroluminescence panel according to any one of claims 1 to 5, wherein the light-transmitting cathode is composed of at least a thin-film metal or alloy.
　７．前記光透過性を有する陰極が、含窒素化合物を用いて構成された下地層と、当該下地層上に、銀又は銀を主成分とした合金で構成されている電極層を有する構成であることを特徴とする第１項から第６項までのいずれか一項に記載の有機エレクトロルミネッセンスパネル。 7. The light-transmitting cathode has an underlayer composed of a nitrogen-containing compound and an electrode layer composed of silver or an alloy containing silver as a main component on the underlayer. The organic electroluminescence panel according to any one of items 1 to 6, wherein:
　８．前記有機エレクトロルミネッセンスパネルと外部電極との接続部は、導電性接着剤により電気的接続されていることを特徴とする第１項から第７項までのいずれか一項に記載の有機エレクトロルミネッセンスパネル。 8. 8. The organic electroluminescence panel according to any one of claims 1 to 7, wherein a connection portion between the organic electroluminescence panel and the external electrode is electrically connected by a conductive adhesive. .
　９．前記複数の有機エレクトロルミネッセンス素子が、ガスバリアー層を有するフレキシブル性樹脂部材により封止されていることを特徴とする第１項から第８項までのいずれか一項に記載の有機エレクトロルミネッセンスパネル。 9. The organic electroluminescence panel according to any one of claims 1 to 8, wherein the plurality of organic electroluminescence elements are sealed with a flexible resin member having a gas barrier layer.
　１０．前記複数の発光エリアが、前記セパレーターにより分離され、ストライプ状に並列配置されていることを特徴とする第１項から第９項までのいずれか一項に記載の有機エレクトロルミネッセンスパネル。 10. The organic electroluminescence panel according to any one of claims 1 to 9, wherein the plurality of light emitting areas are separated by the separator and arranged in parallel in a stripe shape.
　１１．前記外部電極は、光透過性を有するフレキシブルプリント回路から構成されることを特徴とする第８項から第１０項までのいずれか一項に記載の有機エレクトロルミネッセンスパネル。 11. The organic electroluminescence panel according to any one of Items 8 to 10, wherein the external electrode is formed of a flexible printed circuit having light transmittance.
　１２．第１項から第１１項までのいずれか一項に記載の有機エレクトロルミネッセンスパネルを製造する有機エレクトロルミネッセンスパネルの製造方法であって、
　非発光時の波長５５０ｎｍにおける光透過率が５０％以上である有機エレクトロルミネッセンス素子を有し、
　当該有機エレクトロルミネッセンス素子において、基材上に、少なくとも陽極、有機機能層ユニット及び陰極より構成される発光エリアを、複数に分割して形成し、
　前記陰極を、前記陽極上に設けたセパレーターにより分離したパターンを形成し、
　分割されている一方の発光エリアを構成する陽極を、隣接する他方の発光エリアを構成する陰極と、直列に電気的に接続し、
　かつ、前記陽極、陰極及びセパレーターを、フォトリソグラフィー法により形成することを特徴とする有機エレクトロルミネッセンスパネルの製造方法。 12 It is a manufacturing method of the organic electroluminescent panel which manufactures the organic electroluminescent panel as described in any one of Claim 1 to 11,
Having an organic electroluminescence device having a light transmittance of 50% or more at a wavelength of 550 nm when not emitting light,
In the organic electroluminescence element, on the base material, a light emitting area composed of at least an anode, an organic functional layer unit and a cathode is divided into a plurality of parts,
Forming a pattern in which the cathode is separated by a separator provided on the anode;
The anode constituting one light emitting area that is divided is electrically connected in series with the cathode constituting the other neighboring light emitting area,
And the said anode, a cathode, and a separator are formed by the photolithographic method, The manufacturing method of the organic electroluminescent panel characterized by the above-mentioned.
　１３．前記陽極と前記セパレーターとの間に、フォトリソグラフィー法を用いて絶縁層を形成することを特徴とする第１２項に記載の有機エレクトロルミネッセンスパネルの製造方法。 13. 13. The method for manufacturing an organic electroluminescence panel according to item 12, wherein an insulating layer is formed between the anode and the separator using a photolithography method.
　本発明によれば、複数の分割された発光エリアより構成される広い発光面積を有し、輝度均一性及び安定性が向上した有機エレクトロルミネッセンスパネル及びその製造方法を提供することができる。 According to the present invention, it is possible to provide an organic electroluminescence panel having a wide light emitting area composed of a plurality of divided light emitting areas and having improved luminance uniformity and stability, and a method for manufacturing the same.
　本発明で規定する構成からなる有機エレクトロルミネッセンスパネルの技術的特徴とその効果の発現機構は、以下のように推察される。 The technical features of the organic electroluminescence panel having the configuration defined in the present invention and the mechanism of its effects are inferred as follows.
　通常、光透過性を有する有機エレクトロルミネッサンス素子を大面積化しようとした場合、供給する電流量が大きいため、給電端からパネル中央部にかけての陽極もしくは陰極の電圧降下の影響が大きく、輝度ムラが発生する問題があった。 Normally, when trying to increase the area of an organic electroluminescent element having optical transparency, the amount of current supplied is large, so the influence of the voltage drop of the anode or cathode from the feeding end to the center of the panel is large, resulting in uneven brightness. There was a problem that occurred.
　本発明の有機エレクトロルミネッサンスパネルでは、発光エリアを複数に分割し（分割数をＮとする。）、一方の発光エリアを構成する陽極が、他方の発光エリアを構成する陰極と、直列に電気的に接続することにより、必要な電流をＩ／Ｎに低減することで、給電端からパネル中央部までの陽極もしくは陰極の電圧降下も、Ｉ／Ｎに低減する。それにより、発光均一性に優れた大面積の有機エレクトロルミネッセンスパネルの実現が可能となった。 In the organic electroluminescence panel of the present invention, the light emitting area is divided into a plurality of parts (the number of divisions is N), and the anode constituting one light emitting area is electrically connected in series with the cathode constituting the other light emitting area. By connecting them to each other, the required current is reduced to I / N, so that the voltage drop of the anode or cathode from the feed end to the center of the panel is also reduced to I / N. As a result, it became possible to realize a large-area organic electroluminescence panel with excellent emission uniformity.
本発明に適用可能な有機ＥＬ素子の構成の一例を示す概略断面図Schematic sectional view showing an example of the configuration of an organic EL element applicable to the present invention 本発明の有機ＥＬパネルの構成の一例を示す概略断面図（実施形態１）Schematic sectional view showing an example of the configuration of the organic EL panel of the present invention (Embodiment 1) 本発明の有機ＥＬパネルの構成で、絶縁層を有する一例を示す概略断面図（実施形態２）Schematic sectional view showing an example having an insulating layer in the configuration of the organic EL panel of the present invention (Embodiment 2) 本発明の有機ＥＬパネルの構成で、ガスバリアー層を有する構成の一例を示す概略断面図（実施形態３）Schematic sectional view showing an example of a configuration having a gas barrier layer in the configuration of the organic EL panel of the present invention (Embodiment 3) 複数の発光エリアをストライプ状に配置した有機ＥＬパネルの上面図及び概略断面図（実施形態４）A top view and a schematic cross-sectional view of an organic EL panel in which a plurality of light emitting areas are arranged in a stripe pattern (Embodiment 4) 比較例の有機ＥＬパネルの回路構成の一例を示す概略回路図Schematic circuit diagram showing an example of the circuit configuration of an organic EL panel of a comparative example 本発明の有機ＥＬパネルの回路構成の一例を示す概略回路図Schematic circuit diagram showing an example of the circuit configuration of the organic EL panel of the present invention 本発明の有機ＥＬパネルの構成で、封止部材を設けた構成の一例を示す概略断面図（実施形態５）Schematic sectional view showing an example of a configuration in which a sealing member is provided in the configuration of the organic EL panel of the present invention (Embodiment 5) 図７で示す実施形態５の有機ＥＬパネルの作製手順の一例を示す工程フロー図（実施形態６）Process flow diagram showing an example of a manufacturing procedure of the organic EL panel of Embodiment 5 shown in FIG. 7 (Embodiment 6) 本発明に適用可能な有機ＥＬ素子の構成の他の一例を示す概略断面図（実施形態７）Schematic sectional view showing another example of the configuration of the organic EL element applicable to the present invention (Embodiment 7) 本発明に適用可能な有機ＥＬ素子の構成の他の一例を示す概略断面図（実施形態８）Schematic sectional view showing another example of the configuration of an organic EL element applicable to the present invention (Embodiment 8) 本発明に適用可能な有機ＥＬパネルと外部電極との電気的接続方法の一例を示す概略図（実施態様９）Schematic which shows an example of the electrical connection method of the organic electroluminescent panel and external electrode which can be applied to this invention (embodiment 9)
　本発明の有機エレクトロルミネッセンスパネルは、非発光時の波長５５０ｎｍにおける光透過率が５０％以上である有機エレクトロルミネッセンス素子を有し、前記有機エレクトロルミネッセンス素子は、基材上に、少なくとも陽極、有機機能層ユニット及び陰極より構成される発光エリアが、複数に分割されており、前記発光エリアを構成する前記陽極及び前記陰極が、いずれも光透過性を有する電極で構成され、前記陰極が、前記陽極上に設けたセパレーターにより分離した構成であり、かつ、分割されている一方の発光エリアを構成する陽極が、隣接する他方の発光エリアを構成する陰極と、直列に電気的に接続されていることを特徴とする。この特徴は、各請求項に係る発明に共通する又は対応する技術的特徴である。 The organic electroluminescence panel of the present invention has an organic electroluminescence element having a light transmittance of 50% or more at a wavelength of 550 nm when not emitting light, and the organic electroluminescence element has at least an anode and an organic function on a substrate. A light emitting area composed of a layer unit and a cathode is divided into a plurality of parts, each of the anode and the cathode constituting the light emitting area is composed of a light-transmitting electrode, and the cathode is the anode. Separated by the separator provided above, and the anode constituting one of the divided light emitting areas is electrically connected in series with the cathode constituting the other neighboring light emitting area It is characterized by. This feature is a technical feature common to or corresponding to the claimed invention.
　本発明の実施形態としては、本発明の目的とする効果をより発現できる観点から、陽極とセパレーターとの間に、更に絶縁層を設ける構成とすることが、より優れた同一発光エリア内での各電極間の絶縁性を更に高めることができ、安定性がより向上することができる観点から好ましい形態である。 As an embodiment of the present invention, from the standpoint that the effects of the present invention can be further manifested, it is preferable that an insulating layer is further provided between the anode and the separator in the same light emitting area. This is a preferable form from the viewpoint that the insulation between the electrodes can be further improved and the stability can be further improved.
　また、基材として、光透過性を有するガラス基材又はフレキシブル性樹脂基材を適用することが、より高い光透過性を実現することができる観点から好ましい形態である。 In addition, it is a preferable form to apply a light-transmitting glass substrate or flexible resin substrate as the substrate from the viewpoint of realizing higher light transmittance.
　また、基材としてフレキシブル性樹脂基材を適用する場合には、フレキシブル性樹脂基材と有機ＥＬ構成層との間にガスバリアー層を形成することが、有機ＥＬ構成層に対する水分や酸素等による影響を排除することができ、高い耐久性を得ることができる観点から好ましい。 In addition, when a flexible resin base material is applied as the base material, a gas barrier layer is formed between the flexible resin base material and the organic EL constituent layer due to moisture, oxygen, or the like with respect to the organic EL constituent layer. It is preferable from the viewpoint that the influence can be eliminated and high durability can be obtained.
　また、光透過性を有する陽極を、酸化物半導体又は薄膜の金属若しくは合金で構成することが、高い光透過性と優れた導電性を両立する電極を得ることができる点で好ましい。 Further, it is preferable that the light-transmitting anode is made of an oxide semiconductor or a thin-film metal or alloy because an electrode having both high light transmittance and excellent conductivity can be obtained.
　また、光透過性を有する陰極が少なくとも薄膜の金属又は合金で構成されていることが、高い光透過性と優れた導電性を両立する電極を得ることができる点で好ましい。 Further, it is preferable that the light-transmitting cathode is composed of at least a thin metal or alloy because an electrode having both high light transmittance and excellent conductivity can be obtained.
　また、光透過性を有する陰極として、銀又は銀を主成分とした合金で構成されている電極層を適用する場合、含窒素化合物を用いて構成された下地層を設け、その上部に当該電極層を形成することが、陰極として、銀原子が凝集等を起こすことなく存在し、均一な薄銀膜を形成することができる観点から好ましい。 Further, when an electrode layer made of silver or an alloy containing silver as a main component is applied as a light-transmitting cathode, a base layer made of a nitrogen-containing compound is provided, and the electrode is formed on the upper layer. It is preferable to form a layer from the viewpoint that, as a cathode, silver atoms are present without causing aggregation or the like, and a uniform thin silver film can be formed.
　また、有機エレクトロルミネッセンスパネルと外部電極との接続部は、導電性接着剤により電気的接続されていることが好ましい形態である。 Further, it is preferable that the connecting portion between the organic electroluminescence panel and the external electrode is electrically connected by a conductive adhesive.
　また、複数の有機エレクトロルミネッセンス素子が、ガスバリアー層を有するフレキシブル性樹脂基材により封止されていることが、有機ＥＬ構成層に対する水分や酸素等による影響を排除することができ、高い耐久性を得ることができる観点から好ましい。 In addition, the fact that a plurality of organic electroluminescence elements are sealed with a flexible resin substrate having a gas barrier layer can eliminate the influence of moisture, oxygen, etc. on the organic EL constituent layer, and has high durability. From the viewpoint that can be obtained.
　また、複数の発光エリアが、ストライプ状に並列配置されていることが、効率よく広い面積を分割することにより、安定した発光特性を得ることができる観点から好ましい。 In addition, it is preferable that a plurality of light emitting areas are arranged in parallel in a stripe shape from the viewpoint of obtaining stable light emission characteristics by efficiently dividing a large area.
　また、外部電極は、光透過性を有するフレキシブルプリント回路から構成されることが、薄膜でかつ光透過性の高い回路設計を行うことができる観点から好ましい形態である。 In addition, it is preferable that the external electrode is composed of a light-transmitting flexible printed circuit from the viewpoint of being able to design a thin film and highly light-transmitting circuit.
　また、本発明の有機エレクトロルミネッセンスパネルの製造方法としては、上記で規定する構成からなる非発光時の波長５５０ｎｍにおける光透過率が５０％以上である有機エレクトロルミネッセンス素子を有し、当該有機エレクトロルミネッセンス素子において、基材上に、少なくとも陽極、有機機能層ユニット及び陰極より構成される発光エリアを、複数に分割して形成し、前記陰極を、前記陽極上に設けたセパレーターにより分離したパターンを形成し、分割されている一方の発光エリアを構成する陽極を、隣接する他方の発光エリアを構成する陰極と、直列に電気的に接続し、かつ、前記陽極、陰極及びセパレーターを、フォトリソグラフィー法により形成することを特徴とする有機エレクトロルミネッセンスパネルの製造方法であることが、高精細で構成パターンを形成でき、狭い非発光エリアを形成することができる有機エレクトロルミネッセンスパネルを製造することができる。 Moreover, as a manufacturing method of the organic electroluminescent panel of this invention, it has the organic electroluminescent element which is 50% or more of the light transmittance in wavelength 550nm at the time of the non-light-emitting which consists of a structure prescribed | regulated above, The said organic electroluminescent In the element, a light emitting area composed of at least an anode, an organic functional layer unit, and a cathode is formed on a substrate by dividing it into a plurality, and a pattern is formed in which the cathode is separated by a separator provided on the anode. Then, the anode constituting one of the divided light emitting areas is electrically connected in series with the cathode constituting the other neighboring light emitting area, and the anode, the cathode and the separator are connected by photolithography. In the manufacturing method of the organic electroluminescent panel characterized by forming Rukoto is possible to form a structure pattern with high precision, it is possible to manufacture an organic electroluminescent panel capable of forming a narrow non-light emitting area.
　また、陽極とセパレーターとの間に、フォトリソグラフィー法を用いて絶縁層を形成することが、高い絶縁性を得ることができるとともに、高精細な絶縁層を形成することができる点で、好ましい形態である。 In addition, it is preferable to form an insulating layer using a photolithography method between the anode and the separator in that a high insulating property can be obtained and a high-definition insulating layer can be formed. It is.
　本発明でいう「有機ＥＬパネル」とは、複数に分割した発光エリアを構成する複数の有機ＥＬ素子を同一平面状に配置し、それぞれ、有機ＥＬ素子の陽極が、隣接する他方の陰極と電気的に接し、大面積の発光体を構成しているものをいう。 In the present invention, the “organic EL panel” refers to a plurality of organic EL elements constituting a light emitting area divided into a plurality of parts arranged in the same plane, and the anode of the organic EL element is electrically connected to the other adjacent cathode. In contact with each other and constituting a large-area light emitter.
　本発明でいう「有機ＥＬ素子」とは、分割した発光エリアを構成する素子で、基材上に、対向する一対の光透過性を有する電極（陽極及び陰極）と、当該光透過性を有する電極間に、主に電子又は正孔の輸送を制御するキャリア輸送機能層と発光層により構成される有機機能層ユニットを有し、更にその上部に封止部材を設けた構成をいう。ただし、説明の都合で、封止部材の記載や説明を省略する場合がある。また、本発明においては、有機ＥＬ素子の発光を制御する制御回路や配線の記載は省略する。 The “organic EL element” as used in the present invention is an element that constitutes a divided light-emitting area, and has a pair of opposed light-transmitting electrodes (anode and cathode) on the base material and the light-transmitting property. A configuration in which an organic functional layer unit mainly composed of a carrier transporting functional layer for controlling the transport of electrons or holes and a light emitting layer is provided between electrodes, and a sealing member is further provided thereon. However, description and description of the sealing member may be omitted for convenience of explanation. In the present invention, description of a control circuit and wiring for controlling light emission of the organic EL element is omitted.
　本発明でいう「有機機能層ユニット」とは、後述の図１で説明するが、一例としては、基材上に、第１のキャリア輸送機能層群１（例えば、正孔注入層、正孔輸送層等）と、リン光性化合物等を含有する発光層と、第２のキャリア輸送機能層群２（例えば、正孔阻止層、電子輸送層、電子注入層等）が積層配置されている構成をいう。 The “organic functional layer unit” in the present invention will be described with reference to FIG. 1 to be described later. As an example, a first carrier transporting functional layer group 1 (for example, a hole injection layer, a hole is formed on a substrate. A transport layer, a light emitting layer containing a phosphorescent compound, and the like, and a second carrier transport function layer group 2 (for example, a hole blocking layer, an electron transport layer, an electron injection layer, and the like) are stacked. Refers to the configuration.
　本発明でいう「発光エリア」とは、層厚方向で、陽極、有機機能層ユニット及び陰極の全ての構成要素が存在している領域をいう。 In the present invention, the “light emitting area” refers to a region where all components of the anode, the organic functional layer unit, and the cathode exist in the layer thickness direction.
　本発明でいう「陽極」とは、電圧として（＋）を印加する電極であり、「アノード」あるいは「第１の電極」という場合がある。また、「陰極」とは、電圧として（－）を印加する電極であり、「カソード」または「第２の電極」という場合がある。 In the present invention, the “anode” is an electrode to which (+) is applied as a voltage, and may be referred to as “anode” or “first electrode”. The “cathode” is an electrode to which (−) is applied as a voltage, and may be referred to as “cathode” or “second electrode”.
　また、本発明でいう「光透過性」とは、波長５５０ｎｍにおける光透過率が５０％以上であることをいい、好ましくは６０％以上であり、さらに好ましくは７０％以上である。 In addition, the “light transmittance” in the present invention means that the light transmittance at a wavelength of 550 nm is 50% or more, preferably 60% or more, and more preferably 70% or more.
　以下、本発明の構成要素、及び本発明を実施するための形態について、図を交えて詳細な説明をする。なお、本願において、数値範囲を表す「～」は、その前後に記載される数値を下限値及び上限値として含む意味で使用している。なお、各図の説明において、構成要素の末尾に括弧内で記載した数字は、各図における符号を表す。 Hereinafter, constituent elements of the present invention and modes for carrying out the present invention will be described in detail with reference to the drawings. In the present application, “˜” representing a numerical range is used in the sense of including the numerical values described before and after the numerical value as the lower limit value and the upper limit value. In the description of each figure, the number described in parentheses at the end of the constituent element represents the code in each figure.
　《有機ＥＬ素子の基本構成》
　はじめに、有機ＥＬ素子の基本的な構成について、図を交えて説明する。 << Basic structure of organic EL element >>
First, the basic configuration of the organic EL element will be described with reference to the drawings.
　本発明の有機ＥＬパネルにおいては、適用する有機ＥＬ素子が、非発光時の波長５５０ｎｍにおける光透過率が５０％以上である両面発光型の有機ＥＬ素子であることを１つの特徴とする。 One feature of the organic EL panel of the present invention is that the applied organic EL element is a double-sided light emitting organic EL element having a light transmittance of 50% or more at a wavelength of 550 nm when not emitting light.
　図１は、本発明に適用可能な有機ＥＬ素子の有機機能層ユニットを含めた基本的な構成を示す概略断面図である。 FIG. 1 is a schematic sectional view showing a basic configuration including an organic functional layer unit of an organic EL element applicable to the present invention.
　図１で示す本発明に係る有機ＥＬ素子（ＯＬＥＤ）は、光透過性を有する基材（１）、例えば、ガラス基材又はフレキシブル性樹脂基材上に、陽極（３）、発光層及びキャリア輸送機能層から構成される有機機能層ユニット（Ｕ）、陰極（７）等を積層した構造を示してある。 The organic EL element (OLED) according to the present invention shown in FIG. 1 is formed on a light-transmitting substrate (1) such as a glass substrate or a flexible resin substrate, an anode (3), a light emitting layer, and a carrier. A structure in which an organic functional layer unit (U) composed of a transport functional layer, a cathode (7), and the like are laminated is shown.
　図１に示す有機ＥＬ素子（ＯＬＥＤ）は、光透過性を有する基材（１）上に、ガスバリアー層（２）を形成している例を示してある。当該ガスバリアー層（２）上に分割して形成する発光エリアにおいては、第１電極として陽極（３）を形成し、陽極（３）の一方の端部（図１の左側）の上部に、セパレーター（８）が設けられている。セパレーター（８）の形状としては、特に制限はなく、矩形状、台形状、逆テーパー形状等が挙げられるが、図１に示すような逆テーパー状のオーバーハング構造であること好ましい。このセパレーター（８）は、隔壁あるいはカソードセパレーターという場合もある。 The organic EL element (OLED) shown in FIG. 1 shows an example in which a gas barrier layer (2) is formed on a light-transmitting substrate (1). In the light emitting area formed separately on the gas barrier layer (2), the anode (3) is formed as the first electrode, and on the upper part of one end (left side in FIG. 1) of the anode (3), A separator (8) is provided. There is no restriction | limiting in particular as a shape of a separator (8), Although rectangular shape, trapezoid shape, reverse taper shape, etc. are mentioned, It is preferable that it is an overhang structure of reverse taper shape as shown in FIG. This separator (8) may be called a partition or a cathode separator.
　一方、陽極（３）のセパレーター（８）を形成した以外の領域上に、例えば、正孔注入層、正孔輸送層等から構成される第１のキャリア輸送機能層群１（４）、発光層（５）及び、例えば、電子輸送層、電子注入層等から構成される第２のキャリア輸送機能層群２（６）を積層して、有機機能層ユニット（Ｕ）を構成している。 On the other hand, on the region other than the anode (3) where the separator (8) is formed, for example, a first carrier transporting functional layer group 1 (4) composed of a hole injection layer, a hole transporting layer, etc., light emission The organic functional layer unit (U) is configured by laminating the layer (5) and the second carrier transport functional layer group 2 (6) composed of, for example, an electron transport layer, an electron injection layer, and the like.
　更に、一方の有機ＥＬ素子（ＯＬＥＤ）と隣接する他方の有機ＥＬ素子のそれぞれのセパレーター（８）間には、独立したパターンで、第２電極として、陰極（７）が設けられている。そして、上記説明した構成の積層体全体を被覆する形で、封止用接着層（９）及びガスバリアー層（１０）を有する封止基板（１１）が設けられて、有機ＥＬ素子（ＯＬＥＤ）を構成している。この時、分割されている一方の発光エリアを構成する陽極（３）が、隣接する他方の発光エリアを構成する陰極（３）と、直列に電気的に接続されている。 Furthermore, a cathode (7) is provided as a second electrode between the separators (8) of one organic EL element (OLED) and the other adjacent organic EL element in an independent pattern. And the sealing board | substrate (11) which has the contact bonding layer (9) and a gas barrier layer (10) is provided in the form which coat | covers the whole laminated body of the structure demonstrated above, and an organic EL element (OLED) Is configured. At this time, the anode (3) constituting one divided light emitting area is electrically connected in series with the cathode (3) constituting the other adjacent light emitting area.
　本発明においては、図１に示す構成において、第１電極である陽極（３）及び第２電極である陰極（７）が、いずれも波長５５０ｎｍにおける光透過率が５０％以上である電極であることを１つの特徴とする。 In the present invention, in the configuration shown in FIG. 1, the anode (3) as the first electrode and the cathode (7) as the second electrode are both electrodes having a light transmittance of 50% or more at a wavelength of 550 nm. This is one feature.
　このように陽極及び陰極の双方を、光透過性を有する電極で構成することにより、有機機能層ユニットの発光層又はその界面で発光した発光光（Ｌ）を、光透過性を有する第１電極（３）側である基材（１）面の発光エリア及び、同じく光透過性を有する第２電極（７）側の封止部材（１１）面側の発光エリアより外部に発光光（Ｌ）を取り出すことができる。 Thus, by constituting both the anode and the cathode with an electrode having optical transparency, the emitted light (L) emitted from the light emitting layer of the organic functional layer unit or its interface is used as the first electrode having optical transparency. (3) The emitted light (L) is emitted from the light emitting area on the substrate (1) surface which is the side and the light emitting area on the sealing electrode (11) side on the second electrode (7) side which is also light transmissive. Can be taken out.
　発光エリアとは、図１で示すように、陽極（３）と、有機機能層ユニット（Ｕ）、特には発光層（５）と、陰極（７）の全ての構成要素が、同一面上に存在する領域をいう。 As shown in FIG. 1, the light emitting area means that all components of the anode (3), the organic functional layer unit (U), particularly the light emitting layer (5), and the cathode (7) are on the same plane. An area that exists.
　本発明の有機ＥＬパネルにおいては、基材上に、少なくとも陽極（８）、有機機能層ユニット（Ｕ）及び陰極（７）より構成される発光エリアが、セパレーター（８）を介して、複数に分割されて配置されていて、分割されている一方の発光エリアを構成する陽極が、隣接する他方の発光エリアを構成する陰極と、直列に電気的に接続されていることを１つの特徴とする。詳しくは、図１で示すように、「ＯＬＥＤの１構成単位」として示す有機ＥＬ素子（ＯＬＥＤ）を構成する陽極（３）が、左側に配置（詳細な記載は省略）されている陰極（７）と電気的に接続され、かつ「「ＯＬＥＤの１構成単位」として示す有機ＥＬ素子（ＯＬＥＤ）の陰極（７）が、右側に配置（詳細な構成の記載は省略してある。）されている陽極（３）と電気的に接続されている構成で、複数個存在する発光エリア（有機ＥＬ素子）が直列に接続されている構成であることを特徴とする。 In the organic EL panel of the present invention, a plurality of light-emitting areas composed of at least the anode (8), the organic functional layer unit (U), and the cathode (7) are provided on the substrate via the separator (8). One feature is that the anodes that are divided and arranged so that one of the divided light emitting areas is electrically connected in series with the cathode that constitutes the other adjacent light emitting area. . Specifically, as shown in FIG. 1, an anode (3) constituting an organic EL element (OLED) shown as "one constituent unit of OLED" is disposed on the left side (detailed description is omitted) (7 ) And the cathode (7) of the organic EL element (OLED) shown as “one constituent unit of OLED” is arranged on the right side (detailed configuration is omitted). A structure in which a plurality of light emitting areas (organic EL elements) are connected in series with a structure electrically connected to the anode (3).
　また、本発明に係る有機ＥＬ素子においては、２つ以上の有機機能層ユニットを積層したタンデム型構成としてもよい。 Moreover, the organic EL element according to the present invention may have a tandem configuration in which two or more organic functional layer units are stacked.
　本発明の有機ＥＬパネルにおいては、この様に、セパレーター（８）を介して、発光エリアを複数に分割し、分割されている一方の発光エリアを構成する陽極を、隣接する他方の発光エリアを構成する陰極と、直列に電気的に接続する構成とすることにより、発光に必要な電流値を低減し、輝度均一性に優れた大面積の有機ＥＬパネルを実現することができた。 Thus, in the organic EL panel of the present invention, the light emitting area is divided into a plurality of parts via the separator (8), and the anode constituting one of the divided light emitting areas is used as the other adjacent light emitting area. By configuring the cathode to be electrically connected in series, the current value required for light emission was reduced, and a large-area organic EL panel excellent in luminance uniformity could be realized.
　［有機ＥＬ素子の構成要素］
　はじめに、本発明の有機ＥＬパネルを構成する有機ＥＬ素子の主要構成要素の詳細について説明する。 [Components of organic EL element]
First, the detail of the main component of the organic EL element which comprises the organic EL panel of this invention is demonstrated.
　本発明に係る光透過性を有する有機ＥＬ素子（ＯＬＥＤ）は、前述の図１における説明と重複するが、ガスバリアー層（２）を有する基板（１）上に、第１電極である光透過性を有する陽極（３）を当該ガスバリアー層（２）上の分割してある領域に、第１電極として陽極（３）を形成し、陽極（３）の一方の端部（図１の左側）の上部に、逆台形のセパレーター（８）が設けられている。 The light-transmitting organic EL element (OLED) according to the present invention overlaps with the description in FIG. 1 described above, but the light transmission as the first electrode on the substrate (1) having the gas barrier layer (2). The anode (3) having the property is formed as a first electrode in a region divided on the gas barrier layer (2), and one end of the anode (3) (the left side in FIG. 1) ) Is provided with an inverted trapezoidal separator (8).
　次いで、陽極（３）のセパレーター（８）を形成した以外の領域上に、例えば、正孔注入層、正孔輸送層等から構成されるキャリア輸送機能層群１（４）、発光層（５）、例えば、電子輸送層、電子注入層等から構成されるキャリア輸送機能層群２（６）が積層されて、発光領域を構成している。そして、さらに上部の一対のセパレーター（８）により分離されている領域に、第２電極である光透過性を有する陰極（７）が形成され、その上に封止用接着層（９）及びガスバリアー層（１０）を有する封止基板（１１）が設けられている。 Next, on the region of the anode (3) other than where the separator (8) is formed, for example, a carrier transport function layer group 1 (4) composed of a hole injection layer, a hole transport layer, and the like, a light emitting layer (5) ), For example, a carrier transport functional layer group 2 (6) composed of an electron transport layer, an electron injection layer, and the like is laminated to form a light emitting region. Further, a light-transmitting cathode (7) as a second electrode is formed in a region separated by the pair of upper separators (8), and a sealing adhesive layer (9) and a gas are formed thereon. A sealing substrate (11) having a barrier layer (10) is provided.
　以下に、有機ＥＬ素子の構成の代表例を示す。 The following is a typical example of the configuration of the organic EL element.
　（ｉ）光透過性を有する陽極（３）／セパレーター（８）／有機機能層ユニット（Ｕ）〔キャリア輸送機能層群１（４：正孔注入輸送層）／発光層（５）／キャリア輸送機能層群２（６：電子注入輸送層）〕／光透過性を有する陰極（７）
　（ii）光透過性を有する陽極（３）／セパレーター（８）／有機機能層ユニット（Ｕ）〔キャリア輸送機能層群１（４：正孔注入輸送層）／発光層（５）／キャリア輸送機能層群２（６：正孔阻止層／電子注入輸送層）〕／光透過性を有する陰極（７）
　（iii）光透過性を有する陽極（３）／セパレーター（８）／有機機能層ユニット（Ｕ）〔キャリア輸送機能層群１（４：正孔注入輸送層／電子阻止層）／発光層（５）／キャリア輸送機能層群２（６：正孔阻止層／電子注入輸送層）〕／光透過性を有する陰極（７）
　（iv）光透過性を有する陽極（３）／セパレーター（８）／有機機能層ユニット（Ｕ）〔キャリア輸送機能層群１（４：正孔注入層／正孔輸送層）／発光層（５）／キャリア輸送機能層群２（６：電子輸送層／電子注入層）〕／光透過性を有する陰極（７）
　（ｖ）光透過性を有する陽極（３）／セパレーター（８）／有機機能層ユニット（Ｕ）〔キャリア輸送機能層群１（４：正孔注入層／正孔輸送層）／発光層（５）／キャリア輸送機能層群２（６：正孔阻止層／電子輸送層／電子注入層）〕／光透過性を有する陰極（７）
　（vi）光透過性を有する陽極（３）／セパレーター（８）／有機機能層ユニット（Ｕ）〔キャリア輸送機能層群１（４：正孔注入層／正孔輸送層／電子阻止層）／発光層（５）／キャリア輸送機能層群２（６：正孔阻止層／電子輸送層／電子注入層）〕／光透過性を有する陰極（７）
　更に、上記構成に加えて、陽極（３）とセパレーター（８）との間には、後述する絶縁層（１２）を設ける構成も、好ましい形態である。 (I) Light-transmitting anode (3) / separator (8) / organic functional layer unit (U) [carrier transport functional layer group 1 (4: hole injection transport layer) / light emitting layer (5) / carrier transport Functional layer group 2 (6: electron injecting and transporting layer)] / cathode having optical transparency (7)
(Ii) Light-transmitting anode (3) / separator (8) / organic functional layer unit (U) [carrier transport functional layer group 1 (4: hole injection transport layer) / light emitting layer (5) / carrier transport Functional layer group 2 (6: hole blocking layer / electron injecting and transporting layer)] / cathode having optical transparency (7)
(Iii) Light-transmitting anode (3) / separator (8) / organic functional layer unit (U) [carrier transport functional layer group 1 (4: hole injection transport layer / electron blocking layer) / light emitting layer (5 ) / Carrier transporting functional layer group 2 (6: hole blocking layer / electron injection transporting layer)] / cathode having optical transparency (7)
(Iv) Light-transmitting anode (3) / separator (8) / organic functional layer unit (U) [carrier transport functional layer group 1 (4: hole injection layer / hole transport layer) / light emitting layer (5 ) / Carrier transporting functional layer group 2 (6: electron transporting layer / electron injecting layer)] / cathode having optical transparency (7)
(V) Light-transmitting anode (3) / separator (8) / organic functional layer unit (U) [carrier transport functional layer group 1 (4: hole injection layer / hole transport layer) / light emitting layer (5) ) / Carrier transport functional layer group 2 (6: hole blocking layer / electron transport layer / electron injection layer)] / cathode having optical transparency (7)
(Vi) Light-transmitting anode (3) / separator (8) / organic functional layer unit (U) [carrier transport functional layer group 1 (4: hole injection layer / hole transport layer / electron blocking layer) / Light emitting layer (5) / carrier transport functional layer group 2 (6: hole blocking layer / electron transport layer / electron injection layer)] / light-transmitting cathode (7)
Furthermore, in addition to the above configuration, a configuration in which an insulating layer (12) described later is provided between the anode (3) and the separator (8) is also a preferable mode.
　本発明に適用可能な有機ＥＬ素子の概要については、例えば、特開２０１３－１５７６３４号公報、特開２０１３－１６８５５２号公報、特開２０１３－１７７３６１号公報、特開２０１３－１８７２１１号公報、特開２０１３－１９１６４４号公報、特開２０１３－１９１８０４号公報、特開２０１３－２２５６７８号公報、特開２０１３－２３５９９４号公報、特開２０１３－２４３２３４号公報、特開２０１３－２４３２３６号公報、特開２０１３－２４２３６６号公報、特開２０１３－２４３３７１号公報、特開２０１３－２４５１７９号公報、特開２０１４－００３２４９号公報、特開２０１４－００３２９９号公報、特開２０１４－０１３９１０号公報、特開２０１４－０１７４９３号公報、特開２０１４－０１７４９４号公報等に記載されている構成を挙げることができる。 As for the outline of the organic EL element applicable to the present invention, for example, JP2013-157634A, JP2013-168552A, JP2013-177361A, JP2013-187221A, JP JP 2013-191644 A, JP 2013-191804 A, JP 2013-225678 A, JP 2013-235994 A, JP 2013-243234 A, JP 2013-243236 A, JP 2013-2013 A. JP 242366, JP 2013-243371, JP 2013-245179, JP 2014-003249, JP 2014-003299, JP 2014-013910, JP 2014-017493. Gazette, JP 2014-017494 A It can be mentioned configurations described in equal.
　また、タンデム型の有機ＥＬ素子とすることもでき、タンデム型の具体例としては、例えば、米国特許第６３３７４９２号明細書、米国特許第７４２０２０３号明細書、米国特許第７４７３９２３号明細書、米国特許第６８７２４７２号明細書、米国特許第６１０７７３４号明細書、米国特許第６３３７４９２号明細書、国際公開第２００５／００９０８７号、特開２００６－２２８７１２号公報、特開２００６－２４７９１号公報、特開２００６－４９３９３号公報、特開２００６－４９３９４号公報、特開２００６－４９３９６号公報、特開２０１１－９６６７９号公報、特開２００５－３４０１８７号公報、特許第４７１１４２４号公報、特許第３４９６６８１号公報、特許第３８８４５６４号公報、特許第４２１３１６９号公報、特開２０１０－１９２７１９号公報、特開２００９－０７６９２９号公報、特開２００８－０７８４１４号公報、特開２００７－０５９８４８号公報、特開２００３－２７２８６０号公報、特開２００３－０４５６７６号公報、国際公開第２００５／０９４１３０号等に記載の素子構成や構成材料等が挙げられるが、本発明はこれらに限定されない。 A tandem organic EL element can also be used. Specific examples of the tandem type include, for example, US Pat. No. 6,337,492, US Pat. No. 7,420,203, US Pat. No. 7,473,923, US Pat. No. 6,872,472, US Pat. No. 6,107,734, US Pat. No. 6,337,492, WO 2005/009087, JP 2006-228712, JP 2006-24791, JP 2006- No. 49393, JP-A-2006-49394, JP-A-2006-49396, JP-A-2011-96679, JP-A-2005-340187, JP-A-4711424, JP-A-3496681, Patent No. No. 3884564, Japanese Patent No. 431169, JP 2010-192719, JP 2009-076929, JP 2008-078414, JP 2007-059848, JP 2003-272860, JP 2003-045676, International Publication No. Examples of element configurations and constituent materials described in JP 2005/094130 A, and the like are included, but the present invention is not limited thereto.
　更に、有機ＥＬ素子の各構成要素の詳細について説明する。 Further, details of each component of the organic EL element will be described.
　〔基材〕
　有機ＥＬ素子（ＯＬＥＤ）に適用可能な基材（１）としては、光透過性を有する基材であれば特に制限はなく、例えば、ガラス、樹脂基材等の種類を挙げることができる。 〔Base material〕
The substrate (1) applicable to the organic EL element (OLED) is not particularly limited as long as it is a light-transmitting substrate, and examples thereof include glass and resin substrates.
　本発明に適用可能な光透過性を有する基材（１）としては、ガラス、石英、樹脂基材を挙げることができるが、更に好ましくは、有機ＥＬ素子にフレキシブル性を付与することができる観点からフレキシブル性樹脂基材である。 Examples of the light-transmitting substrate (1) applicable to the present invention include glass, quartz, and a resin substrate. More preferably, the organic EL element can be provided with flexibility. To flexible resin base material.
　本発明に適用可能な樹脂基材を構成する樹脂材料としては、例えば、ポリエチレンテレフタレート（略称：ＰＥＴ）、ポリエチレンナフタレート（略称：ＰＥＮ）等のポリエステル、ポリエチレン、ポリプロピレン、セロファン、セルロースジアセテート、セルローストリアセテート（略称：ＴＡＣ）、セルロースアセテートブチレート、セルロースアセテートプロピオネート（略称：ＣＡＰ）、セルロースアセテートフタレート、セルロースナイトレート等のセルロースエステル類及びそれらの誘導体、ポリ塩化ビニリデン、ポリビニルアルコール、ポリエチレンビニルアルコール、シンジオタクティックポリスチレン、ポリカーボネート（略称：ＰＣ）、ノルボルネン樹脂、ポリメチルペンテン、ポリエーテルケトン、ポリイミド、ポリエーテルスルホン（略称：ＰＥＳ）、ポリフェニレンスルフィド、ポリスルホン類、ポリエーテルイミド、ポリエーテルケトンイミド、ポリアミド、フッ素樹脂、ナイロン、ポリメチルメタクリレート、アクリル及びポリアリレート類、アートン（商品名、ＪＳＲ社製）及びアペル（商品名、三井化学社製）等のシクロオレフィン系樹脂等を挙げることができる。 Examples of the resin material constituting the resin base material applicable to the present invention include polyesters such as polyethylene terephthalate (abbreviation: PET), polyethylene naphthalate (abbreviation: PEN), polyethylene, polypropylene, cellophane, cellulose diacetate, and cellulose. Cellulose esters such as triacetate (abbreviation: TAC), cellulose acetate butyrate, cellulose acetate propionate (abbreviation: CAP), cellulose acetate phthalate, cellulose nitrate, and their derivatives, polyvinylidene chloride, polyvinyl alcohol, polyethylene vinyl alcohol , Syndiotactic polystyrene, polycarbonate (abbreviation: PC), norbornene resin, polymethylpentene, polyetherketone, polyimide, Ether sulfone (abbreviation: PES), polyphenylene sulfide, polysulfones, polyether imide, polyether ketone imide, polyamide, fluororesin, nylon, polymethyl methacrylate, acrylic and polyarylates, Arton (trade name, manufactured by JSR) and Examples thereof include cycloolefin resins such as Apel (trade name, manufactured by Mitsui Chemicals).
　これら樹脂基材のうち、コストや入手の容易性の点から、ポリエチレンテレフタレート（略称：ＰＥＴ）、ポリブチレンテレフタレート、ポリエチレンナフタレート（略称：ＰＥＮ）、ポリカーボネート（略称：ＰＣ）等のフレキシブル性を有する樹脂基材が好ましく用いることができる。 Among these resin base materials, from the viewpoint of cost and availability, polyethylene terephthalate (abbreviation: PET), polybutylene terephthalate, polyethylene naphthalate (abbreviation: PEN), polycarbonate (abbreviation: PC), etc. have flexibility. A resin base material can be preferably used.
　また、上記の樹脂基材は、未延伸フィルムでもよく、延伸フィルムでもよい。 The resin substrate may be an unstretched film or a stretched film.
　本発明に適用可能な樹脂基材は、従来公知の製膜方法により製造することが可能である。例えば、材料となる樹脂を押出機により溶融し、環状ダイやＴダイにより押し出して急冷することにより、実質的に無定形で配向していない未延伸の樹脂基材を製造することができる。また、樹脂成分を溶媒に溶解してドープを調製した後、当該ドープを金属支持体上に流延、乾燥して成膜する溶液流延法により製造した樹脂基材も適用することができる。また、未延伸の樹脂基材を一軸延伸、テンター式逐次二軸延伸、テンター式同時二軸延伸、チューブラー式同時二軸延伸等の公知の方法により、樹脂基材の搬送方向（縦軸方向、ＭＤ方向）、又は樹脂基材の搬送方向と直角の方向（横軸方向、ＴＤ方向）に延伸することにより、延伸樹脂基材を製造することができる。この場合の延伸倍率は、樹脂基材の原料となる樹脂に合わせて適宜選択することできるが、縦軸方向及び横軸方向にそれぞれ１．０１～１０倍の範囲内であることが好ましい。 The resin base material applicable to the present invention can be manufactured by a conventionally known film forming method. For example, an unstretched resin base material that is substantially amorphous and not oriented can be produced by melting a resin as a material with an extruder, extruding it with an annular die or a T-die, and quenching. A resin substrate produced by a solution casting method in which a resin component is dissolved in a solvent to prepare a dope and then the dope is cast on a metal support and dried to form a film can also be applied. In addition, the unstretched resin base material is transported in the direction of the resin base material (vertical axis direction) by a known method such as uniaxial stretching, tenter sequential biaxial stretching, tenter simultaneous biaxial stretching, tubular simultaneous biaxial stretching, or the like. , MD direction), or a stretched resin substrate can be produced by stretching in a direction perpendicular to the conveying direction of the resin substrate (horizontal axis direction, TD direction). The draw ratio in this case can be appropriately selected according to the resin as the raw material of the resin base material, but is preferably in the range of 1.01 to 10 times in the vertical axis direction and the horizontal axis direction.
　樹脂基材は、厚さとして３～２００μｍの範囲内にある薄膜の樹脂基材であることが好ましいが、より好ましくは１０～１５０μｍの範囲内であり、特に好ましくは、２０～１２０μｍの範囲内である。 The resin substrate is preferably a thin film resin substrate having a thickness in the range of 3 to 200 μm, more preferably in the range of 10 to 150 μm, and particularly preferably in the range of 20 to 120 μm. It is.
　また、本発明に係る光透過性を有する基材として適用可能なガラス基材としては、ソーダ石灰ガラス、バリウム・ストロンチウム含有ガラス、鉛ガラス、アルミノケイ酸ガラス、ホウケイ酸ガラス、バリウムホウケイ酸ガラス、石英等を挙げることができる。 Further, as a glass substrate applicable as a light-transmitting substrate according to the present invention, soda lime glass, barium / strontium-containing glass, lead glass, aluminosilicate glass, borosilicate glass, barium borosilicate glass, quartz Etc.
　〔第１電極：光透過性を有する陽極〕
　有機ＥＬ素子を構成する光透過性を有する陽極としては、酸化物半導体又は薄膜の金属若しくは合金で構成されていることが好ましい形態であり、例えば、Ａｇ、Ａｕ等の金属又は金属を主成分とする合金、ＣｕＩ、あるいはインジウム・スズの複合酸化物（ＩＴＯ）、ＳｎＯ２及びＺｎＯ等の酸化物半導体を挙げることができる。 [First electrode: anode having optical transparency]
The light-transmitting anode constituting the organic EL element is preferably composed of an oxide semiconductor or a thin-film metal or alloy, for example, a metal such as Ag or Au or a metal as a main component. And oxide semiconductors such as CuI, indium-tin composite oxide (ITO), SnO 2 and ZnO.
　光透過性を有する陽極を、銀を主成分として構成する場合、銀の純度としては、９９％以上であることが好ましい。また、銀の安定性を確保するためにパラジウム（Ｐｄ）、銅（Ｃｕ）及び金（Ａｕ）等が添加されていてもよい。 When the light-transmitting anode is composed mainly of silver, the purity of silver is preferably 99% or more. Further, palladium (Pd), copper (Cu), gold (Au), or the like may be added to ensure the stability of silver.
　光透過性を有する陽極は、銀を主成分として構成されている層とすることができるが、具体的には、銀単独で形成しても、あるいは銀（Ａｇ）を含有する合金から構成されていてもよい。そのような合金としては、例えば、銀・マグネシウム（Ａｇ・Ｍｇ）、銀・銅（Ａｇ・Ｃｕ）、銀・パラジウム（Ａｇ・Ｐｄ）、銀・パラジウム・銅（Ａｇ・Ｐｄ・Ｃｕ）、銀・インジウム（Ａｇ・Ｉｎ）などが挙げられる。 The light-transmitting anode can be a layer composed mainly of silver. Specifically, the anode can be formed of silver alone or an alloy containing silver (Ag). It may be. Examples of such alloys include silver / magnesium (Ag / Mg), silver / copper (Ag / Cu), silver / palladium (Ag / Pd), silver / palladium / copper (Ag / Pd / Cu), silver -Indium (Ag.In) etc. are mentioned.
　上記陽極を構成する各構成材料の中でも、本発明に係る有機ＥＬ素子を構成する陽極としては、銀を主成分として構成し、厚さが２～２０ｎｍの範囲内にある光透過性を有する陽極であることが好ましいが、更に好ましくは厚さが４～１２ｎｍの範囲内である。厚さが２０ｎｍ以下であれば、光透過性を有する陽極の吸収成分及び反射成分が低く抑えられ、高い光透過率が維持されるため好ましい。 Among the constituent materials constituting the anode, as the anode constituting the organic EL device according to the present invention, an anode having a light transmission property composed mainly of silver and having a thickness in the range of 2 to 20 nm. The thickness is preferably in the range of 4 to 12 nm. A thickness of 20 nm or less is preferable because the absorption component and reflection component of the light-transmitting anode are kept low and high light transmittance is maintained.
　本発明でいう銀を主成分として構成されている層とは、光透過性を有する陽極中の銀の含有量が６０質量％以上であることをいい、好ましくは銀の含有量が８０質量％以上であり、より好ましくは銀の含有量が９０質量％以上であり、特に好ましくは銀の含有量が９８質量％以上である。また、本発明に係る光透過性を有する陽極でいう「光透過性」とは、波長５５０ｎｍでの光透過率が５０％以上であることをいう。 The layer composed mainly of silver in the present invention means that the silver content in the light-transmitting anode is 60% by mass or more, preferably the silver content is 80% by mass. More preferably, the silver content is 90% by mass or more, and particularly preferably the silver content is 98% by mass or more. Further, “light transmittance” in the anode having light transmittance according to the present invention means that the light transmittance at a wavelength of 550 nm is 50% or more.
　光透過性を有する陽極においては、銀を主成分として構成されている層が、必要に応じて複数の層に分けて積層された構成であっても良い。 The light-transmitting anode may have a structure in which a layer composed mainly of silver is divided into a plurality of layers as necessary.
　また、本発明においては、陽極が、銀を主成分として構成する光透過性を有する陽極である場合には、形成する光透過性を有する陽極の銀膜の均一性を高める観点から、その下部に、下地層を設けることが好ましい。下地層としては、特に制限はないが、窒素原子又は硫黄原子を有する有機化合物を含有する層であることが好ましく、当該下地層上に、銀を主成分として光透過性を有する陽極を形成する方法が好ましい態様である。なお、本発明に適用可能な下地層の詳細については後述する。 In the present invention, when the anode is a light-transmitting anode composed mainly of silver, the lower portion is formed from the viewpoint of improving the uniformity of the silver film of the light-transmitting anode to be formed. It is preferable to provide an underlayer. Although there is no restriction | limiting in particular as a base layer, It is preferable that it is a layer containing the organic compound which has a nitrogen atom or a sulfur atom, and forms the anode which has a light transmittance which has silver as a main component on the said base layer. The method is a preferred embodiment. The details of the underlayer applicable to the present invention will be described later.
　〔セパレーター〕
　本発明においては、各有機ＥＬ素子間にセパレーターを設け、陰極が、陽極上に設けた２つのセパレーターにより分離した構成であることを特徴とする。 〔separator〕
The present invention is characterized in that a separator is provided between each organic EL element, and the cathode is separated by two separators provided on the anode.
　本発明に係るセパレーターは、陽極の長手方向と直交する方向にストライプ状に形成される。このセパレーターは、絶縁性を有しており、陰極を複数のエリアに分割する機能を有するものである。 The separator according to the present invention is formed in a stripe shape in a direction perpendicular to the longitudinal direction of the anode. This separator has an insulating property and has a function of dividing the cathode into a plurality of areas.
　パッシブ型の光透過性を有する有機ＥＬ素子の場合、通常、陽極がストライプ状に形成されることから、このストライプ状の陽極の長手方向に直交するように、セパレーターもストライプ状に形成される。 In the case of an organic EL element having passive light transmittance, since the anode is usually formed in a stripe shape, the separator is also formed in a stripe shape so as to be orthogonal to the longitudinal direction of the stripe-shaped anode.
　セパレーターが所定の高さを有していれば、陰極を複数のエリアに分割することができるため、セパレーターの断面形状としては、特に限定されるものではなく、例えば、矩形状、台形状（順テーパー形状）、逆テーパー形状等が挙げられる。好ましくは、図１で示すような逆テーパー状のオーバーハング構造である。 If the separator has a predetermined height, the cathode can be divided into a plurality of areas. Therefore, the cross-sectional shape of the separator is not particularly limited. For example, a rectangular shape, a trapezoidal shape (in order) Taper shape), reverse taper shape and the like. A reverse taper overhang structure as shown in FIG. 1 is preferable.
　セパレーターが逆テーパー形状の場合、基材あるいは陽極表面に対するテーパー角度θは、０°＜θ＜９０°であればよいが、好ましくは２０°＜θ＜８０°、より好ましくは３０°＜θ＜７０°である。 When the separator has a reverse taper shape, the taper angle θ with respect to the substrate or the anode surface may be 0 ° <θ <90 °, preferably 20 ° <θ <80 °, more preferably 30 ° <θ <. 70 °.
　セパレーターの高さとしては、通常、セパレーターの下地である陽極あるいは絶縁層表面からセパレーター表面までの高さが、発光領域の中心部における基材（１）表面から陰極（７）表面までの高さよりも高くなるように設定される。 As the height of the separator, the height from the surface of the anode or the insulating layer, which is the base of the separator, to the surface of the separator is usually higher than the height from the surface of the substrate (1) to the surface of the cathode (7) at the center of the light emitting region. Is set to be higher.
　セパレーターの幅は、特に限定されるものではないが、１００μｍ以下であることが好ましい。セパレーターの幅が広すぎると、発光領域が相対的に狭くなり、発光面積が低下するため好ましくない。 The width of the separator is not particularly limited, but is preferably 100 μm or less. If the width of the separator is too wide, the light emitting region becomes relatively narrow and the light emitting area is reduced, which is not preferable.
　セパレーターのピッチは、特に限定されるものではなく、目的とする有機ＥＬ素子の画素の大きさ等によって、適宜選択されるものである。 The pitch of the separator is not particularly limited, and is appropriately selected depending on the pixel size of the target organic EL element.
　セパレーターの構成材料としては、例えば、感光性ポリイミド樹脂、アクリル系樹脂、ノボラック系樹脂、スチレン系樹脂、フェノール系樹脂、メラミン系樹脂等の光硬化型樹脂、または熱硬化型樹脂、および無機材料等を挙げることができる。 As a constituent material of the separator, for example, a photosensitive polyimide resin, an acrylic resin, a novolac resin, a styrene resin, a phenol resin, a photocurable resin such as a melamine resin, or a thermosetting resin, an inorganic material, etc. Can be mentioned.
　セパレーターの形成方法としては、フォトリソグラフィー法、印刷法等の一般的な方法を挙げることができるが、本発明の有機エレクトロルミネッセンスパネルの製造方法においては、フォトリソグラフィー法により形成することを特徴とする。フォトリソグラフィー法によるセパレーターの形成方法の詳細ついては後述する。 Examples of the method for forming the separator include general methods such as a photolithography method and a printing method. In the method for producing an organic electroluminescence panel of the present invention, the separator is formed by a photolithography method. . Details of the method for forming the separator by photolithography will be described later.
　〔発光層〕
　有機ＥＬ素子（ＯＬＥＤ）を構成する発光層（５）は、発光材料としてリン光発光化合物、あるいは蛍光性化合物を用いることができるが、本発明においては、特に、発光材料としてリン光発光化合物が含有されている構成が好ましい。 [Light emitting layer]
In the light emitting layer (5) constituting the organic EL element (OLED), a phosphorescent light emitting compound or a fluorescent compound can be used as the light emitting material. In the present invention, in particular, a phosphorescent light emitting compound is used as the light emitting material. The contained structure is preferable.
　この発光層は、電極又は電子輸送層から注入された電子と、正孔輸送層から注入された正孔とが再結合して発光する層であり、発光する部分は発光層の層内領域であっても発光層と隣接する層との界面領域であってもよい。 This light emitting layer is a layer that emits light by recombination of electrons injected from the electrode or the electron transport layer and holes injected from the hole transport layer, and the light emitting portion is an in-layer region of the light emitting layer. Even the interface region between the light emitting layer and the adjacent layer may be used.
　このような発光層としては、含まれる発光材料が発光要件を満たしていれば、その構成には特に制限はない。また、同一の発光スペクトルや発光極大波長を有する層が複数層あってもよい。この場合、各発光層間には非発光性の中間層を有していることが好ましい。 Such a light emitting layer is not particularly limited in its configuration as long as the light emitting material contained satisfies the light emission requirements. Moreover, there may be a plurality of layers having the same emission spectrum and emission maximum wavelength. In this case, it is preferable to have a non-light emitting intermediate layer between the light emitting layers.
　発光層の厚さの総和は、１～１００ｎｍの範囲内にあることが好ましく、より低い駆動電圧を得ることができることから１～３０ｎｍの範囲内がさらに好ましい。なお、発光層の厚さの総和とは、発光層間に非発光性の中間層が存在する場合には、当該中間層も含む厚さである。 The total thickness of the light emitting layers is preferably in the range of 1 to 100 nm, and more preferably in the range of 1 to 30 nm because a lower driving voltage can be obtained. In addition, the sum total of the thickness of a light emitting layer is the thickness also including the said intermediate | middle layer, when a nonluminous intermediate | middle layer exists between light emitting layers.
　以上のような発光層は、後述する発光材料やホスト化合物を、例えば、真空蒸着法、スピンコート法、キャスト法、ＬＢ法（ラングミュア・ブロジェット、Ｌａｎｇｍｕｉｒ　Ｂｌｏｄｇｅｔｔ法）及びインクジェット法等の公知の方法により形成することができる。 The light emitting layer as described above is prepared by using a known method such as a vacuum evaporation method, a spin coating method, a casting method, an LB method (Langmuir-Blodget, Langmuir Blodgett method) and an ink jet method. Can be formed.
　また発光層は、複数の発光材料を混合してもよく、リン光発光材料と蛍光発光材料（蛍光ドーパント、蛍光性化合物ともいう）とを同一発光層中に混合して用いてもよい。発光層の構成としては、ホスト化合物（発光ホスト等ともいう）及び発光材料（発光ドーパント化合物ともいう。）を含有し、発光材料より発光させることが好ましい。 In the light emitting layer, a plurality of light emitting materials may be mixed, and a phosphorescent light emitting material and a fluorescent light emitting material (also referred to as a fluorescent dopant or a fluorescent compound) may be mixed and used in the same light emitting layer. The structure of the light-emitting layer preferably includes a host compound (also referred to as a light-emitting host) and a light-emitting material (also referred to as a light-emitting dopant compound), and emits light from the light-emitting material.
　〈ホスト化合物〉
　発光層に含有されるホスト化合物としては、室温（２５℃）におけるリン光発光のリン光量子収率が０．１未満の化合物が好ましい。さらにリン光量子収率が０．０１未満であることが好ましい。また、発光層に含有される化合物の中で、その層中での体積比が５０％以上であることが好ましい。 <Host compound>
As the host compound contained in the light emitting layer, a compound having a phosphorescence quantum yield of phosphorescence emission at room temperature (25 ° C.) of less than 0.1 is preferable. Further, the phosphorescence quantum yield is preferably less than 0.01. Moreover, it is preferable that the volume ratio in the layer is 50% or more among the compounds contained in a light emitting layer.
　ホスト化合物としては、公知のホスト化合物を単独で用いてもよく、あるいは、複数種のホスト化合物を用いてもよい。ホスト化合物を複数種用いることで、電荷の移動を調整することが可能であり、有機ＥＬ素子を高効率化することができる。また、後述する発光材料を複数種用いることで、異なる発光を混ぜることが可能となり、これにより任意の発光色を得ることができる。 As the host compound, a known host compound may be used alone, or a plurality of types of host compounds may be used. By using a plurality of types of host compounds, it is possible to adjust the movement of charges, and the organic EL element can be made highly efficient. In addition, by using a plurality of kinds of light emitting materials described later, it is possible to mix different light emission, thereby obtaining an arbitrary light emission color.
　発光層に用いられるホスト化合物としては、従来公知の低分子化合物でも、繰り返し単位をもつ高分子化合物でもよく、ビニル基やエポキシ基のような重合性基を有する低分子化合物（蒸着重合性発光ホスト）でもよい。 The host compound used in the light emitting layer may be a conventionally known low molecular compound or a high molecular compound having a repeating unit, and a low molecular compound having a polymerizable group such as a vinyl group or an epoxy group (evaporation polymerizable light emitting host). )
　本発明に適用可能なホスト化合物としては、例えば、特開２００１－２５７０７６号公報、同２００１－３５７９７７号公報、同２００２－８８６０号公報、同２００２－４３０５６号公報、同２００２－１０５４４５号公報、同２００２－３５２９５７号公報、同２００２－２３１４５３号公報、同２００２－２３４８８８号公報、同２００２－２６０８６１号公報、同２００２－３０５０８３号公報、米国特許出願公開第２００５／０１１２４０７号明細書、米国特許出願公開第２００９／００３０２０２号明細書、国際公開第２００１／０３９２３４号、国際公開第２００８／０５６７４６号、国際公開第２００５／０８９０２５号、国際公開第２００７／０６３７５４号、国際公開第２００５／０３０９００号、国際公開第２００９／０８６０２８号、国際公開第２０１２／０２３９４７号、特開２００７－２５４２９７号公報、欧州特許第２０３４５３８号明細書等に記載されている化合物を挙げることができる。 Examples of host compounds applicable to the present invention include, for example, JP-A Nos. 2001-257076, 2001-357777, 2002-8860, 2002-43056, 2002-105445, 2002-352957, 2002-231453, 2002-234888, 2002-260861, 2002-305083, US Patent Application Publication No. 2005/0112407, US Patent Application Publication No. 2009/0030202, International Publication No. 2001/039234, International Publication No. 2008/056746, International Publication No. 2005/089025, International Publication No. 2007/063754, International Publication No. 2005/030900, International Publication 200th / No. 086,028, WO 2012/023947, can be mentioned JP 2007-254297, JP-European compounds described in Japanese Patent No. 2034538 Pat like.
　〈発光材料〉
　本発明で用いることのできる発光材料としては、リン光発光性化合物（リン光性化合物、リン光発光材料又はリン光発光ドーパントともいう。）及び蛍光発光性化合物（蛍光性化合物又は蛍光発光材料ともいう。）が挙げられるが、特に、リン光発光性化合物を用いることが、高い発光効率を得ることができる観点から好ましい。 <Light emitting material>
As the light-emitting material that can be used in the present invention, a phosphorescent compound (also referred to as a phosphorescent compound, a phosphorescent material, or a phosphorescent dopant) and a fluorescent compound (both a fluorescent compound or a fluorescent material) are used. In particular, it is preferable to use a phosphorescent compound from the viewpoint of obtaining high luminous efficiency.
　〈リン光発光性化合物〉
　リン光発光性化合物とは、励起三重項からの発光が観測される化合物であり、具体的には室温（２５℃）にてリン光発光する化合物であり、リン光量子収率が２５℃において０．０１以上の化合物であると定義されるが、好ましいリン光量子収率は０．１以上である。 <Phosphorescent compound>
A phosphorescent compound is a compound in which light emission from an excited triplet is observed. Specifically, it is a compound that emits phosphorescence at room temperature (25 ° C.), and the phosphorescence quantum yield is 0 at 25 ° C. A preferred phosphorescence quantum yield is 0.1 or more, although it is defined as 0.01 or more compounds.
　上記リン光量子収率は、第４版実験化学講座７の分光IIの３９８頁（１９９２年版、丸善）に記載の方法により測定できる。溶液中でのリン光量子収率は、種々の溶媒を用いて測定できるが、本発明においてリン光発光性化合物を用いる場合、任意の溶媒のいずれかにおいて、上記リン光量子収率として０．０１以上が達成されればよい。 The phosphorescent quantum yield can be measured by the method described in Spectroscopic II, page 398 (1992 edition, Maruzen) of the Fourth Edition Experimental Chemistry Course 7. The phosphorescence quantum yield in the solution can be measured using various solvents, but when using a phosphorescent compound in the present invention, the phosphorescence quantum yield is 0.01 or more in any solvent. Should be achieved.
　リン光発光性化合物は、一般的な有機ＥＬ素子の発光層に使用される公知のものの中から適宜選択して用いることができるが、好ましくは元素の周期表で８～１０族の金属を含有する錯体系化合物であり、さらに好ましくはイリジウム化合物、オスミウム化合物、白金化合物（白金錯体系化合物）又は希土類錯体であり、中でも最も好ましいのはイリジウム化合物である。 The phosphorescent compound can be appropriately selected from known compounds used for the light-emitting layer of a general organic EL device, but preferably contains a group 8 to 10 metal in the periodic table of elements. More preferred are iridium compounds, more preferred are iridium compounds, osmium compounds, platinum compounds (platinum complex compounds) or rare earth complexes, and most preferred are iridium compounds.
　本発明においては、少なくとも一つの発光層が、二種以上のリン光発光性化合物が含有されていてもよく、発光層におけるリン光発光性化合物の濃度比が発光層の厚さ方向で変化している態様であってもよい。 In the present invention, at least one light emitting layer may contain two or more phosphorescent compounds, and the concentration ratio of the phosphorescent compound in the light emitting layer varies in the thickness direction of the light emitting layer. It may be an embodiment.
　本発明に使用できる公知のリン光発光性化合物の具体例としては、以下の文献に記載されている化合物等が挙げられる。 Specific examples of known phosphorescent compounds that can be used in the present invention include compounds described in the following documents.
　Ｎａｔｕｒｅ　３９５，１５１（１９９８）、Ａｐｐｌ．Ｐｈｙｓ．Ｌｅｔｔ．７８，　１６２２（２００１）、Ａｄｖ．Ｍａｔｅｒ．１９，７３９（２００７）、Ｃｈｅｍ．Ｍａｔｅｒ．１７，３５３２（２００５）、Ａｄｖ．Ｍａｔｅｒ．１７，１０５９（２００５）、国際公開第２００９／１００９９１号、国際公開第２００８／１０１８４２号、国際公開第２００３／０４０２５７号、米国特許出願公開第２００６／８３５４６９号明細書、米国特許出願公開第２００６／０２０２１９４号明細書、米国特許出願公開第２００７／００８７３２１号明細書、米国特許出願公開第２００５／０２４４６７３号明細書等に記載の化合物を挙げることができる。 Nature 395, 151 (1998), Appl. Phys. Lett. 78, 1622 (2001), Adv. Mater. 19, 739 (2007), Chem. Mater. 17, 3532 (2005), Adv. Mater. 17, 1059 (2005), International Publication No. 2009/100991, International Publication No. 2008/101842, International Publication No. 2003/040257, US Patent Application Publication No. 2006/835469, US Patent Application Publication No. 2006 /. Examples thereof include compounds described in US Patent No. 0202194, US Patent Application Publication No. 2007/0087321, US Patent Application Publication No. 2005/0244673, and the like.
　また、Ｉｎｏｒｇ．Ｃｈｅｍ．４０，１７０４（２００１）、Ｃｈｅｍ．Ｍａｔｅｒ．１６，２４８０（２００４）、Ａｄｖ．Ｍａｔｅｒ．１６，２００３（２００４）、Ａｎｇｅｗ．Ｃｈｅｍ．ｌｎｔ．Ｅｄ．２００６，４５，７８００、Ａｐｐｌ．Ｐｈｙｓ．Ｌｅｔｔ．８６，１５３５０５（２００５）、Ｃｈｅｍ．Ｌｅｔｔ．３４，５９２（２００５）、Ｃｈｅｍ．Ｃｏｍｍｕｎ．２９０６（２００５）、Ｉｎｏｒｇ．Ｃｈｅｍ．４２，１２４８（２００３）、国際公開第２００９／０５０２９０号、国際公開第２００９／０００６７３号、米国特許第７３３２２３２号明細書、米国特許出願公開第２００９／００３９７７６号、米国特許第６６８７２６６号明細書、米国特許出願公開第２００６／０００８６７０号明細書、米国特許出願公開第２００８／００１５３５５号明細書、米国特許第７３９６５９８号明細書、米国特許出願公開第２００３／０１３８６５７号明細書、米国特許第７０９０９２８号明細書等に記載の化合物を挙げることができる。 Also, Inorg. Chem. 40, 1704 (2001), Chem. Mater. 16, 2480 (2004), Adv. Mater. 16, 2003 (2004), Angew. Chem. lnt. Ed. 2006, 45, 7800, Appl. Phys. Lett. 86, 153505 (2005), Chem. Lett. 34, 592 (2005), Chem. Commun. 2906 (2005), Inorg. Chem. 42, 1248 (2003), International Publication No. 2009/050290, International Publication No. 2009/000673, US Pat. No. 7,332,232, US Patent Application Publication No. 2009/0039776, US Pat. No. 6,687,266, US Patent Application Publication No. 2006/0008670, US Patent Application Publication No. 2008/0015355, US Pat. No. 7,396,598, US Patent Application Publication No. 2003/0138667, US Pat. No. 7090928 And the like.
　また、Ａｎｇｅｗ．Ｃｈｅｍ．ｌｎｔ．Ｅｄ．４７，１（２００８）、Ｃｈｅｍ．Ｍａｔｅｒ．１８，５１１９（２００６）、Ｉｎｏｒｇ．Ｃｈｅｍ．４６，４３０８（２００７）、Ｏｒｇａｎｏｍｅｔａｌｌｉｃｓ　２３，３７４５（２００４）、Ａｐｐｌ．Ｐｈｙｓ．Ｌｅｔｔ．７４，１３６１（１９９９）、国際公開第２００６／０５６４１８号、国際公開第２００５／１２３８７３号、国際公開第２００５／１２３８７３号、国際公開第２００６／０８２７４２号、米国特許出願公開第２００５／０２６０４４１号明細書、米国特許第７５３４５０５号明細書、米国特許出願公開第２００７／０１９０３５９号明細書、米国特許第７３３８７２２号明細書、米国特許第７２７９７０４号明細書、米国特許出願公開第２００６／１０３８７４号明細書等に記載の化合物も挙げることができる。 Also, Angew. Chem. lnt. Ed. 47, 1 (2008), Chem. Mater. 18, 5119 (2006), Inorg. Chem. 46, 4308 (2007), Organometallics 23, 3745 (2004), Appl. Phys. Lett. 74, 1361 (1999), International Publication No. 2006/056418, International Publication No. 2005/123873, International Publication No. 2005/123873, International Publication No. 2006/082742, US Patent Application Publication No. 2005/0260441. , U.S. Pat. No. 7,534,505, U.S. Patent Application Publication No. 2007/0190359, U.S. Pat. No. 7,338,722, U.S. Pat. No. 7,279,704, U.S. Patent Application Publication No. 2006/103874, etc. Mention may also be made of the compounds described.
　さらには、国際公開第２００５／０７６３８０号、国際公開第２００８／１４０１１５号、国際公開第２０１１／１３４０１３号、国際公開第２０１０／０８６０８９号、国際公開第２０１２／０２０３２７号、国際公開第２０１１／０５１４０４号、国際公開第２０１１／０７３１４９号、特開２００９－１１４０８６号公報、特開２００３－８１９８８号公報、特開２００２－３６３５５２号公報等に記載の化合物も挙げることができる。 Furthermore, International Publication No. 2005/076380, International Publication No. 2008/140115, International Publication No. 2011/134013, International Publication No. 2010/086089, International Publication No. 2012/020327, International Publication No. 2011/051404. Further, compounds described in International Publication No. 2011/073149, JP2009-114086, JP2003-81988, JP2002-363552, and the like can also be mentioned.
　本発明においては、好ましいリン光発光性化合物としてはＩｒを中心金属に有する有機金属錯体が挙げられる。さらに好ましくは、金属－炭素結合、金属－窒素結合、金属－酸素結合、金属－硫黄結合の少なくとも１つの配位様式を含む錯体が好ましい。 In the present invention, preferred phosphorescent compounds include organometallic complexes having Ir as a central metal. More preferably, a complex containing at least one coordination mode of a metal-carbon bond, a metal-nitrogen bond, a metal-oxygen bond, and a metal-sulfur bond is preferable.
　上記説明したリン光発光性化合物（リン光発光性金属錯体ともいう）は、例えば、Ｏｒｇａｎｉｃ　Ｌｅｔｔｅｒ誌、ｖｏｌ３、Ｎｏ．１６、２５７９～２５８１頁（２００１）、Ｉｎｏｒｇａｎｉｃ　Ｃｈｅｍｉｓｔｒｙ，第３０巻、第８号、１６８５～１６８７頁（１９９１年）、Ｊ．Ａｍ．Ｃｈｅｍ．Ｓｏｃ．，１２３巻、４３０４頁（２００１年）、Ｉｎｏｒｇａｎｉｃ　Ｃｈｅｍｉｓｔｒｙ，第４０巻、第７号、１７０４～１７１１頁（２００１年）、Ｉｎｏｒｇａｎｉｃ　Ｃｈｅｍｉｓｔｒｙ，第４１巻、第１２号、３０５５～３０６６頁（２００２年）、Ｎｅｗ　Ｊｏｕｒｎａｌ　ｏｆ　Ｃｈｅｍｉｓｔｒｙ．，第２６巻、１１７１頁（２００２年）、Ｅｕｒｏｐｅａｎ　Ｊｏｕｒｎａｌ　ｏｆ　Ｏｒｇａｎｉｃ　Ｃｈｅｍｉｓｔｒｙ，第４巻、６９５～７０９頁（２００４年）、さらにこれらの文献中に記載されている参考文献等に開示されている方法を適用することにより合成することができる。 The phosphorescent compound described above (also referred to as a phosphorescent metal complex) is described in, for example, Organic Letter, vol. 16, 2579-2581 (2001), Inorganic Chemistry, Vol. 30, No. 8, pp. 1685-1687 (1991), J. Am. Am. Chem. Soc. , 123, 4304 (2001), Inorganic Chemistry, Vol. 40, No. 7, pages 1704-1711 (2001), Inorganic Chemistry, Vol. 41, No. 12, pages 3055-3066 (2002) , New Journal of Chemistry. 26, 1171 (2002), European Journal of Organic Chemistry, Vol. 4, pages 695-709 (2004), and methods disclosed in the references and the like described in these documents Can be synthesized.
　〈蛍光発光性化合物〉
　蛍光発光性化合物としては、クマリン系色素、ピラン系色素、シアニン系色素、クロコニウム系色素、スクアリウム系色素、オキソベンツアントラセン系色素、フルオレセイン系色素、ローダミン系色素、ピリリウム系色素、ペリレン系色素、スチルベン系色素、ポリチオフェン系色素又は希土類錯体系蛍光体等が挙げられる。 <Fluorescent compound>
Fluorescent compounds include coumarin dyes, pyran dyes, cyanine dyes, croconium dyes, squalium dyes, oxobenzanthracene dyes, fluorescein dyes, rhodamine dyes, pyrylium dyes, perylene dyes, stilbene dyes. And dyes, polythiophene dyes, and rare earth complex phosphors.
　〔キャリア輸送機能層群〕
　次いで、キャリア輸送機能層群を構成する各層の代表例として、電荷注入層、正孔輸送層、電子輸送層及び阻止層の順に説明する。 [Carrier transport functional group]
Next, a charge injection layer, a hole transport layer, an electron transport layer, and a blocking layer will be described in this order as representative examples of the layers constituting the carrier transport functional layer group.
　（電荷注入層）
　電荷注入層は、駆動電圧低下や発光輝度向上のために、電極と発光層の間に設けられる層のことで、「有機ＥＬ素子とその工業化最前線（１９９８年１１月３０日エヌ・ティー・エス社発行）」の第２編第２章「電極材料」（１２３～１６６頁）にその詳細が記載されており、正孔注入層と電子注入層とがある。 (Charge injection layer)
The charge injection layer is a layer provided between the electrode and the light emitting layer in order to lower the driving voltage and improve the light emission luminance. “The organic EL element and its industrialization front line (November 30, 1998, NT. The details are described in Volume 2, Chapter 2, “Electrode Materials” (pages 123 to 166) of “Part 2” of S Co., Ltd., and there are a hole injection layer and an electron injection layer.
　電荷注入層としては、一般には、正孔注入層であれば、陽極と発光層又は正孔輸送層との間、電子注入層であれば陰極と発光層又は電子輸送層との間に存在させることができるが、本発明においては、光透過性を有する電極に隣接して電荷注入層を配置させることが好まし構成である。また、中間電極で用いられる場合は、隣接する電子注入層及び正孔注入層の少なくとも一方が、本発明の要件を満たしていれば良い。 In general, the charge injection layer is present between the anode and the light emitting layer or the hole transport layer in the case of a hole injection layer, and between the cathode and the light emitting layer or the electron transport layer in the case of an electron injection layer. However, in the present invention, it is preferable to dispose the charge injection layer adjacent to the light-transmitting electrode. When used in an intermediate electrode, it is sufficient that at least one of the adjacent electron injection layer and hole injection layer satisfies the requirements of the present invention.
　正孔注入層は、駆動電圧低下や発光輝度向上のために、光透過性を有する電極である陽極に隣接して配置される層であり、「有機ＥＬ素子とその工業化最前線（１９９８年１１月３０日エヌ・ティー・エス社発行）」の第２編第２章「電極材料」（１２３～１６６頁）に詳細に記載されている。 The hole injection layer is a layer disposed adjacent to the anode, which is a light-transmitting electrode, in order to lower the driving voltage and improve the light emission luminance. The “organic EL element and its industrialization front line (1998 November The details are described in Volume 2, Chapter 2, “Electrode Materials” (pages 123-166) of “Month 30th, NTS Corporation”.
　正孔注入層は、特開平９－４５４７９号公報、同９－２６００６２号公報、同８－２８８０６９号公報等にもその詳細が記載されており、正孔注入層に用いられる材料としては、例えば、ポルフィリン誘導体、フタロシアニン誘導体、オキサゾール誘導体、オキサジアゾール誘導体、トリアゾール誘導体、イミダゾール誘導体、ピラゾリン誘導体、ピラゾロン誘導体、フェニレンジアミン誘導体、ヒドラゾン誘導体、スチルベン誘導体、ポリアリールアルカン誘導体、トリアリールアミン誘導体、カルバゾール誘導体、インドロカルバゾール誘導体、イソインドール誘導体、アントラセンやナフタレン等のアセン系誘導体、フルオレン誘導体、フルオレノン誘導体、及びポリビニルカルバゾール、芳香族アミンを主鎖又は側鎖に導入した高分子材料又はオリゴマー、ポリシラン、導電性ポリマー又はオリゴマー（例えば、ＰＥＤＯＴ（ポリエチレンジオキシチオフェン）：ＰＳＳ（ポリスチレンスルホン酸）、アニリン系共重合体、ポリアニリン、ポリチオフェン等）等が挙げられる。 The details of the hole injection layer are described in JP-A-9-45479, JP-A-9-260062, JP-A-8-288069, etc. Examples of materials used for the hole injection layer include: , Porphyrin derivatives, phthalocyanine derivatives, oxazole derivatives, oxadiazole derivatives, triazole derivatives, imidazole derivatives, pyrazoline derivatives, pyrazolone derivatives, phenylenediamine derivatives, hydrazone derivatives, stilbene derivatives, polyarylalkane derivatives, triarylamine derivatives, carbazole derivatives, Indolocarbazole derivatives, isoindole derivatives, acene derivatives such as anthracene and naphthalene, fluorene derivatives, fluorenone derivatives, polyvinylcarbazole, aromatic amines introduced into the main chain or side chain Child material or oligomer, polysilane, a conductive polymer or oligomer (e.g., PEDOT (polyethylene dioxythiophene): PSS (polystyrene sulfonic acid), aniline copolymers, polyaniline, polythiophene, etc.) and the like can be mentioned.
　トリアリールアミン誘導体としては、α－ＮＰＤ（４，４′－ビス〔Ｎ－（１－ナフチル）－Ｎ－フェニルアミノ〕ビフェニル）に代表されるベンジジン型や、ＭＴＤＡＴＡ（４，４′，４″－トリス〔Ｎ－（３－メチルフェニル）－Ｎ－フェニルアミノ〕トリフェニルアミン）に代表されるスターバースト型、トリアリールアミン連結コア部にフルオレンやアントラセンを有する化合物等が挙げられる。 Examples of the triarylamine derivative include benzidine type represented by α-NPD (4,4′-bis [N- (1-naphthyl) -N-phenylamino] biphenyl), and MTDATA (4,4 ′, 4 ″). Examples include a starburst type represented by -tris [N- (3-methylphenyl) -N-phenylamino] triphenylamine), a compound having fluorene or anthracene in the triarylamine-linked core.
　また、特表２００３－５１９４３２号公報や特開２００６－１３５１４５号公報等に記載されているようなヘキサアザトリフェニレン誘導体も同様に正孔輸送材料として用いることができる。 In addition, hexaazatriphenylene derivatives such as those described in JP-T-2003-519432 and JP-A-2006-135145 can also be used as a hole transport material.
　電子注入層は、駆動電圧低下や発光輝度向上のために、陰極と発光層との間に設けられる層のことであり、陰極が本発明に係る光透過性を有する電極で構成されている場合には、当該光透過性を有する電極に隣接して設けられ、「有機ＥＬ素子とその工業化最前線（１９９８年１１月３０日エヌ・ティー・エス社発行）」の第２編第２章「電極材料」（１２３～１６６頁）に詳細に記載されている。 The electron injection layer is a layer provided between the cathode and the light emitting layer in order to lower the driving voltage and improve the light emission luminance. When the cathode is composed of the light-transmitting electrode according to the present invention Is provided adjacent to the light-transmitting electrode, and “Organic EL element and its forefront of industrialization” (issued on November 30, 1998 by NTT) The electrode material "(pages 123 to 166) is described in detail.
　電子注入層は、特開平６－３２５８７１号公報、同９－１７５７４号公報、同１０－７４５８６号公報等にもその詳細が記載されており、電子注入層に好ましく用いられる材料の具体例としては、ストロンチウムやアルミニウム等に代表される金属、フッ化リチウム、フッ化ナトリウム、フッ化カリウム等に代表されるアルカリ金属化合物、フッ化マグネシウム、フッ化カルシウム等に代表されるアルカリ金属ハライド層、フッ化マグネシウムに代表されるアルカリ土類金属化合物層、酸化モリブデン、酸化アルミニウム等に代表される金属酸化物、リチウム８－ヒドロキシキノレート（Ｌｉｑ）等に代表される金属錯体等が挙げられる。また、本発明における光透過性を有する電極が陰極の場合は、金属錯体等の有機材料が特に好適に用いられる。電子注入層はごく薄い膜であることが望ましく、構成材料にもよるが、その層厚は１ｎｍ～１０μｍの範囲が好ましい。 Details of the electron injection layer are also described in JP-A-6-325871, JP-A-9-17574, JP-A-10-74586, and the like. Specific examples of materials preferably used for the electron injection layer are as follows. Metals represented by strontium and aluminum, alkali metal compounds represented by lithium fluoride, sodium fluoride, potassium fluoride, etc., alkali metal halide layers represented by magnesium fluoride, calcium fluoride, etc. Examples thereof include an alkaline earth metal compound layer typified by magnesium, a metal oxide typified by molybdenum oxide and aluminum oxide, and a metal complex typified by lithium 8-hydroxyquinolate (Liq). Moreover, when the electrode which has the light transmittance in this invention is a cathode, organic materials, such as a metal complex, are used especially suitably. The electron injection layer is preferably a very thin film, and depending on the constituent material, the layer thickness is preferably in the range of 1 nm to 10 μm.
　（正孔輸送層）
　正孔輸送層とは正孔を輸送する機能を有する正孔輸送材料からなり、広い意味で正孔注入層及び電子阻止層も正孔輸送層の機能を有する。正孔輸送層は単層又は複数層設けることができる。 (Hole transport layer)
The hole transport layer is made of a hole transport material having a function of transporting holes. In a broad sense, the hole injection layer and the electron blocking layer also have the function of a hole transport layer. The hole transport layer can be provided as a single layer or a plurality of layers.
　正孔輸送材料としては、正孔の注入又は輸送、電子の障壁性のいずれかを有するものであり、有機物、無機物のいずれであってもよい。例えば、トリアゾール誘導体、オキサジアゾール誘導体、イミダゾール誘導体、ポリアリールアルカン誘導体、ピラゾリン誘導体、ピラゾロン誘導体、フェニレンジアミン誘導体、アリールアミン誘導体、アミノ置換カルコン誘導体、オキサゾール誘導体、スチリルアントラセン誘導体、フルオレノン誘導体、ヒドラゾン誘導体、スチルベン誘導体、シラザン誘導体、アニリン系共重合体、導電性高分子オリゴマー及びチオフェンオリゴマー等が挙げられる。 The hole transport material has any of hole injection or transport and electron barrier properties, and may be either organic or inorganic. For example, triazole derivatives, oxadiazole derivatives, imidazole derivatives, polyarylalkane derivatives, pyrazoline derivatives, pyrazolone derivatives, phenylenediamine derivatives, arylamine derivatives, amino-substituted chalcone derivatives, oxazole derivatives, styrylanthracene derivatives, fluorenone derivatives, hydrazone derivatives, Examples include stilbene derivatives, silazane derivatives, aniline copolymers, conductive polymer oligomers, and thiophene oligomers.
　正孔輸送材料としては、上記のものを使用することができるが、ポルフィリン化合物、芳香族第３級アミン化合物及びスチリルアミン化合物を用いることができ、特に芳香族第３級アミン化合物を用いることが好ましい。 As the hole transport material, those described above can be used, but porphyrin compounds, aromatic tertiary amine compounds and styrylamine compounds can be used, and in particular, aromatic tertiary amine compounds can be used. preferable.
　芳香族第３級アミン化合物及びスチリルアミン化合物の代表例としては、Ｎ，Ｎ，Ｎ′，Ｎ′－テトラフェニル－４，４′－ジアミノフェニル、Ｎ，Ｎ′－ジフェニル－Ｎ，Ｎ′－ビス（３－メチルフェニル）－〔１，１′－ビフェニル〕－４，４′－ジアミン（略称：ＴＰＤ）、２，２－ビス（４－ジ－ｐ－トリルアミノフェニル）プロパン、１，１－ビス（４－ジ－ｐ－トリルアミノフェニル）シクロヘキサン、Ｎ，Ｎ，Ｎ′，Ｎ′－テトラ－ｐ－トリル－４，４′－ジアミノビフェニル、１，１－ビス（４－ジ－ｐ－トリルアミノフェニル）－４－フェニルシクロヘキサン、ビス（４－ジメチルアミノ－２－メチルフェニル）フェニルメタン、ビス（４－ジ－ｐ－トリルアミノフェニル）フェニルメタン、Ｎ，Ｎ′－ジフェニル－Ｎ，Ｎ′－ジ（４－メトキシフェニル）－４，４′－ジアミノビフェニル、Ｎ，Ｎ，Ｎ′，Ｎ′－テトラフェニル－４，４′－ジアミノジフェニルエーテル、４，４′－ビス（ジフェニルアミノ）クオードリフェニル、Ｎ，Ｎ，Ｎ－トリ（ｐ－トリル）アミン、４－（ジ－ｐ－トリルアミノ）－４′－〔４－（ジ－ｐ－トリルアミノ）スチリル〕スチルベン、４－Ｎ，Ｎ－ジフェニルアミノ－（２－ジフェニルビニル）ベンゼン、３－メトキシ－４′－Ｎ，Ｎ－ジフェニルアミノスチルベンゼン及びＮ－フェニルカルバゾール等が挙げられる。 Representative examples of aromatic tertiary amine compounds and styrylamine compounds include N, N, N ′, N′-tetraphenyl-4,4′-diaminophenyl, N, N′-diphenyl-N, N′— Bis (3-methylphenyl)-[1,1′-biphenyl] -4,4′-diamine (abbreviation: TPD), 2,2-bis (4-di-p-tolylaminophenyl) propane, 1,1 -Bis (4-di-p-tolylaminophenyl) cyclohexane, N, N, N ', N'-tetra-p-tolyl-4,4'-diaminobiphenyl, 1,1-bis (4-di-p -Tolylaminophenyl) -4-phenylcyclohexane, bis (4-dimethylamino-2-methylphenyl) phenylmethane, bis (4-di-p-tolylaminophenyl) phenylmethane, N, N'-diphenyl-N N'-di (4-methoxyphenyl) -4,4'-diaminobiphenyl, N, N, N ', N'-tetraphenyl-4,4'-diaminodiphenyl ether, 4,4'-bis (diphenylamino) Quadriphenyl, N, N, N-tri (p-tolyl) amine, 4- (di-p-tolylamino) -4 '-[4- (di-p-tolylamino) styryl] stilbene, 4-N, N -Diphenylamino- (2-diphenylvinyl) benzene, 3-methoxy-4'-N, N-diphenylaminostilbenzene, N-phenylcarbazole and the like.
　正孔輸送層は、上記正孔輸送材料を、例えば、真空蒸着法、スピンコート法、キャスト法、インクジェット法を含む印刷法及びＬＢ法（ラングミュア・ブロジェット、Ｌａｎｇｍｕｉｒ　Ｂｌｏｄｇｅｔｔ法）等の公知の方法により、薄膜化することにより形成することができる。正孔輸送層の層厚については特に制限はないが、通常は５ｎｍ～５μｍ程度、好ましくは５～２００ｎｍの範囲である。この正孔輸送層は、上記材料の一種又は二種以上からなる単層構造であってもよい。 For the hole transport layer, the hole transport material may be formed by a known method such as a vacuum deposition method, a spin coating method, a casting method, a printing method including an ink jet method, and an LB method (Langmuir Brodget, Langmuir Brodgett method). Thus, it can be formed by thinning. The layer thickness of the hole transport layer is not particularly limited, but is usually about 5 nm to 5 μm, preferably 5 to 200 nm. The hole transport layer may have a single layer structure composed of one or more of the above materials.
　また、正孔輸送層の材料に不純物をドープすることにより、ｐ性を高くすることもできる。その例としては、特開平４－２９７０７６号公報、特開２０００－１９６１４０号公報、同２００１－１０２１７５号公報及びＪ．Ａｐｐｌ．Ｐｈｙｓ．，９５，５７７３（２００４）等に記載されたものが挙げられる。 Also, the p property can be increased by doping impurities into the material of the hole transport layer. Examples thereof include JP-A-4-297076, JP-A-2000-196140, 2001-102175 and J.P. Appl. Phys. 95, 5773 (2004), and the like.
　このように、正孔輸送層のｐ性を高くすると、より低消費電力の素子を作製することができるため好ましい。 Thus, it is preferable to increase the p property of the hole transport layer because an element with lower power consumption can be manufactured.
　（電子輸送層）
　電子輸送層は、電子を輸送する機能を有する材料から構成され、広い意味で電子注入層、正孔阻止層も電子輸送層に含まれる。電子輸送層は、単層構造又は複数層の積層構造として設けることができる。 (Electron transport layer)
The electron transport layer is made of a material having a function of transporting electrons, and in a broad sense, an electron injection layer and a hole blocking layer are also included in the electron transport layer. The electron transport layer can be provided as a single layer structure or a stacked structure of a plurality of layers.
　単層構造の電子輸送層及び積層構造の電子輸送層において、発光層に隣接する層部分を構成する電子輸送材料（正孔阻止材料を兼ねる）としては、カソードより注入された電子を発光層に伝達する機能を有していれば良い。このような材料としては、従来公知の化合物の中から任意のものを選択して用いることができる。例えば、ニトロ置換フルオレン誘導体、ジフェニルキノン誘導体、チオピランジオキシド誘導体、カルボジイミド、フレオレニリデンメタン誘導体、アントラキノジメタン、アントロン誘導体及びオキサジアゾール誘導体等が挙げられる。さらに、上記オキサジアゾール誘導体において、オキサジアゾール環の酸素原子を硫黄原子に置換したチアジアゾール誘導体、電子吸引基として知られているキノキサリン環を有するキノキサリン誘導体も、電子輸送層の材料として用いることができる。さらにこれらの材料を高分子鎖に導入した高分子材料又はこれらの材料を高分子の主鎖とした高分子材料を用いることもできる。 In the electron transport layer having a single-layer structure and the electron transport layer having a multilayer structure, an electron transport material (also serving as a hole blocking material) constituting a layer portion adjacent to the light emitting layer is used as an electron transporting material. What is necessary is just to have the function to transmit. As such a material, any one of conventionally known compounds can be selected and used. Examples include nitro-substituted fluorene derivatives, diphenylquinone derivatives, thiopyran dioxide derivatives, carbodiimides, fluorenylidenemethane derivatives, anthraquinodimethane, anthrone derivatives, and oxadiazole derivatives. Furthermore, in the above oxadiazole derivative, a thiadiazole derivative in which the oxygen atom of the oxadiazole ring is substituted with a sulfur atom, and a quinoxaline derivative having a quinoxaline ring known as an electron-withdrawing group can also be used as a material for the electron transport layer. it can. Furthermore, a polymer material in which these materials are introduced into a polymer chain, or a polymer material having these materials as a polymer main chain can also be used.
　また、８－キノリノール誘導体の金属錯体、例えば、トリス（８－キノリノール）アルミニウム（略称：Ａｌｑ３）、トリス（５，７－ジクロロ－８－キノリノール）アルミニウム、トリス（５，７－ジブロモ－８－キノリノール）アルミニウム、トリス（２－メチル－８－キノリノール）アルミニウム、トリス（５－メチル－８－キノリノール）アルミニウム、ビス（８－キノリノール）亜鉛（略称：Ｚｎｑ）等及びこれらの金属錯体の中心金属がＩｎ、Ｍｇ、Ｃｕ、Ｃａ、Ｓｎ、Ｇａ又はＰｂに置き替わった金属錯体も、電子輸送層の材料として用いることができる。 In addition, metal complexes of 8-quinolinol derivatives such as tris (8-quinolinol) aluminum (abbreviation: Alq 3 ), tris (5,7-dichloro-8-quinolinol) aluminum, tris (5,7-dibromo-8- Quinolinol) aluminum, tris (2-methyl-8-quinolinol) aluminum, tris (5-methyl-8-quinolinol) aluminum, bis (8-quinolinol) zinc (abbreviation: Znq), etc. and the central metal of these metal complexes A metal complex replaced with In, Mg, Cu, Ca, Sn, Ga, or Pb can also be used as a material for the electron transport layer.
　電子輸送層は、上記材料を、例えば、真空蒸着法、スピンコート法、キャスト法、インクジェット法を含む印刷法及びＬＢ法等の公知の方法により、薄膜化することで形成することができる。電子輸送層の層厚については特に制限はないが、通常は５ｎｍ～５μｍ程度、好ましくは５～２００ｎｍの範囲内である。電子輸送層は上記材料の一種又は二種以上からなる単層構造であってもよい。 The electron transport layer can be formed by thinning the above material by a known method such as a vacuum deposition method, a spin coating method, a casting method, a printing method including an inkjet method, and an LB method. The thickness of the electron transport layer is not particularly limited, but is usually about 5 nm to 5 μm, preferably 5 to 200 nm. The electron transport layer may have a single layer structure composed of one or more of the above materials.
　（阻止層）
　阻止層としては、正孔阻止層及び電子阻止層が挙げられ、上記説明したキャリア輸送機能層ユニット３の各構成層の他に、必要に応じて設けられる層である。例えば、特開平１１－２０４２５８号公報、同１１－２０４３５９号公報、及び「有機ＥＬ素子とその工業化最前線（１９９８年１１月３０日エヌ・ティー・エス社発行）」の２３７頁等に記載されている正孔阻止（ホールブロック）層等を挙げることができる。 (Blocking layer)
Examples of the blocking layer include a hole blocking layer and an electron blocking layer. In addition to the constituent layers of the carrier transport functional layer unit 3 described above, the blocking layer is a layer provided as necessary. For example, it is described in JP-A Nos. 11-204258 and 11-204359, and “Organic EL elements and the forefront of industrialization (published by NTT Corporation on November 30, 1998)” on page 237. Hole blocking (hole block) layer and the like.
　正孔阻止層とは、広い意味では、電子輸送層の機能を有する。正孔阻止層は、電子を輸送する機能を有しつつ正孔を輸送する能力が著しく小さい正孔阻止材料からなり、電子を輸送しつつ正孔を阻止することで電子と正孔の再結合確率を向上させることができる。また、電子輸送層の構成を必要に応じて、正孔阻止層として用いることができる。正孔阻止層は、発光層に隣接して設けられていることが好ましい。 The hole blocking layer has a function of an electron transport layer in a broad sense. The hole blocking layer is made of a hole blocking material that has a function of transporting electrons but has a very small ability to transport holes, and recombines electrons and holes by blocking holes while transporting electrons. Probability can be improved. Moreover, the structure of an electron carrying layer can be used as a hole-blocking layer as needed. The hole blocking layer is preferably provided adjacent to the light emitting layer.
　一方、電子阻止層とは、広い意味では、正孔輸送層の機能を有する。電子阻止層は、正孔を輸送する機能を有しつつ、電子を輸送する能力が著しく小さい材料からなり、正孔を輸送しつつ電子を阻止することで電子と正孔の再結合確率を向上させることができる。また、正孔輸送層の構成を必要に応じて電子阻止層として用いることができる。本発明に適用する正孔阻止層の層厚としては、好ましくは３～１００ｎｍの範囲であり、さらに好ましくは５～３０ｎｍの範囲である。 On the other hand, the electron blocking layer has a function of a hole transport layer in a broad sense. The electron blocking layer is made of a material that has the ability to transport holes and has a very small ability to transport electrons. By blocking holes while transporting holes, the probability of recombination of electrons and holes is improved. Can be made. Moreover, the structure of a positive hole transport layer can be used as an electron blocking layer as needed. The layer thickness of the hole blocking layer applied to the present invention is preferably in the range of 3 to 100 nm, more preferably in the range of 5 to 30 nm.
　〔第２電極：光透過性を有する陰極〕
　本発明に係るセパレーターにより分割して構成される陰極は、キャリア輸送機能層群や発光層に正孔を供給するために機能する光透過性を有する電極であり、金属、合金、有機又は無機の導電性化合物若しくはこれらの混合物として、例えば、金、アルミニウム、銀、マグネシウム、リチウム、マグネシウム／銅混合物、マグネシウム／銀混合物、マグネシウム／アルミニウム混合物、マグネシウム／インジウム混合物、インジウム、リチウム／アルミニウム混合物、希土類金属、ＩＴＯ、ＺｎＯ、ＴｉＯ２及びＳｎＯ２等の酸化物半導体などが挙げられるが、その中でも、少なくとも薄膜の金属又は合金で構成されていることが好ましい構成であり、さらに好ましくは、含窒素化合物を用いて構成された下地層と、当該下地層上に、銀又は銀を主成分とした合金で構成されている電極層を有する構成であることが好ましい。 [Second electrode: Cathode having optical transparency]
The cathode constituted by dividing the separator according to the present invention is a light-transmitting electrode that functions to supply holes to the carrier transporting functional layer group and the light emitting layer, and is made of metal, alloy, organic or inorganic Examples of conductive compounds or mixtures thereof include gold, aluminum, silver, magnesium, lithium, magnesium / copper mixtures, magnesium / silver mixtures, magnesium / aluminum mixtures, magnesium / indium mixtures, indium, lithium / aluminum mixtures, rare earth metals In addition, oxide semiconductors such as ITO, ZnO, TiO 2, and SnO 2 can be used. Among them, it is preferable that the semiconductor is composed of at least a thin-film metal or alloy, more preferably a nitrogen-containing compound. An underlayer composed of Is preferably silver is configured to have an electrode layer is composed of the main component and the alloy.
　光透過性を有する陰極として好適な銀又は銀を主成分とした合金とは、上記陽極の説明で記載したのと同様の材料を挙げることができ、具体的には、銀単独で形成しても、あるいは銀（Ａｇ）を含有する合金から構成されていてもよい。そのような合金としては、例えば、銀・マグネシウム（Ａｇ・Ｍｇ）、銀・銅（Ａｇ・Ｃｕ）、銀・パラジウム（Ａｇ・Ｐｄ）、銀・パラジウム・銅（Ａｇ・Ｐｄ・Ｃｕ）、銀・インジウム（Ａｇ・Ｉｎ）などが挙げられる。 Examples of suitable silver or an alloy containing silver as a main component as a light-transmitting cathode include the same materials as those described in the description of the anode. Alternatively, it may be made of an alloy containing silver (Ag). Examples of such alloys include silver / magnesium (Ag / Mg), silver / copper (Ag / Cu), silver / palladium (Ag / Pd), silver / palladium / copper (Ag / Pd / Cu), silver -Indium (Ag.In) etc. are mentioned.
　陰極は、これらの導電性材料を蒸着やスパッタリング等の方法により薄膜を形成させて作製することができる。また、第２電極としてのシート抵抗は、数百Ω／ｓｑ．以下が好ましく、膜厚は通常５ｎｍ～５μｍ、好ましくは５～２００ｎｍの範囲で選ばれる。 The cathode can be produced by forming a thin film of these conductive materials by a method such as vapor deposition or sputtering. The sheet resistance as the second electrode is several hundred Ω / sq. The film thickness is usually selected from the range of 5 nm to 5 μm, preferably 5 to 200 nm.
　《有機ＥＬパネルの基本構成》
　次いで、本発明の有機ＥＬパネルの詳細について説明する。 << Basic configuration of organic EL panel >>
Next, details of the organic EL panel of the present invention will be described.
　本発明の有機ＥＬパネルにおいては、複数の発光エリア（有機ＥＬ素子）に分割された構成を有し、分割されている一方の発光エリアを構成する陽極が、隣接する他方の発光エリアを構成する陰極と、直列に電気的に接続されている構成であることを特徴とする。 The organic EL panel of the present invention has a structure divided into a plurality of light emitting areas (organic EL elements), and an anode constituting one of the divided light emitting areas constitutes the other adjacent light emitting area. The structure is characterized in that it is electrically connected in series with the cathode.
　以下、複数の分割した発光エリアを有する本発明の有機ＥＬパネルの基本的な構成について説明する。 Hereinafter, a basic configuration of the organic EL panel of the present invention having a plurality of divided light emitting areas will be described.
　〔実施形態１〕
　図２は、複数の有機ＥＬ素子を具備した本発明の有機ＥＬパネルの構成の一例を示す概略断面図（実施形態１）である。 Embodiment 1
FIG. 2 is a schematic cross-sectional view (Embodiment 1) showing an example of the configuration of the organic EL panel of the present invention having a plurality of organic EL elements.
　図２に示す有機ＥＬパネル（Ｐ）では、上記図１で説明した有機ＥＬ素子（ＯＬＥＤ）の構成材料のうち、ガスバリアー層、封止用接着層及び封止部材等の記載は省略してある。 In the organic EL panel (P) shown in FIG. 2, among the constituent materials of the organic EL element (OLED) described in FIG. 1, description of the gas barrier layer, the sealing adhesive layer, the sealing member, and the like is omitted. is there.
　図２に示す有機ＥＬパネル（Ｐ）では、一枚の広い面積を有する光透過性を有する基材（１）上に、複数の有機ＥＬ素子（ＯＬＥＤ）をそれぞれ離間した状態で配置して、独立した発光エリアを形成している。詳しくは、基材（１）上に、陽極（３）、セパレーター（８）、有機機能層ユニット（Ｕ）及び陰極（７）等により構成されている有機ＥＬ素子（ＯＬＥＤ）を複数個配置している。２つのセパレーター（８）間に陰極（７）が電気的に分割した状態で形成され、分割されている一方の発光エリアを構成する陰極（７）が、円形の破線部で示す領域で、隣接する他方の発光エリアを構成する陽極（３）の端部と、直列に電気的に接続した構成を有している。このような構成とすることにより、複数個の有機ＥＬ素子（ＯＬＥＤ）を直列に接続することができる。 In the organic EL panel (P) shown in FIG. 2, a plurality of organic EL elements (OLEDs) are arranged in a state of being separated from each other on a single transparent substrate (1) having a large area, An independent light emitting area is formed. Specifically, a plurality of organic EL elements (OLED) composed of an anode (3), a separator (8), an organic functional layer unit (U), a cathode (7), etc. are arranged on the substrate (1). ing. The cathode (7) is formed in an electrically divided state between the two separators (8), and the cathode (7) constituting one of the divided light emitting areas is adjacent to the area indicated by the circular broken line portion. The other light emitting area is configured to be electrically connected in series with the end of the anode (3) constituting the other light emitting area. By setting it as such a structure, a some organic EL element (OLED) can be connected in series.
　図２に示す構成においては、陰極（７）のセパレーター（８）に接している左端部から陽極（３）の右端部までの領域が「発光エリア」となり、陽極（３）の右端部から隣接する他方の有機ＥＬ素子（ＯＬＥＤ）のセパレーター（８）に接している陰極（７）の左端部までが「非発光エリア」となる。 In the configuration shown in FIG. 2, the area from the left end of the cathode (7) in contact with the separator (8) to the right end of the anode (3) is the “light emitting area”, and is adjacent to the right end of the anode (3). The other end of the cathode (7) in contact with the separator (8) of the other organic EL element (OLED) is the “non-light emitting area”.
　〔実施形態２：絶縁層の形成〕
　本発明の有機ＥＬパネル(Ｐ)においては、陽極（３）とセパレーター（８）との間に、絶縁層（１２）を設けることが、好ましい形態である。 [Embodiment 2: Formation of insulating layer]
In the organic EL panel (P) of the present invention, it is preferable to provide an insulating layer (12) between the anode (3) and the separator (8).
　図３は、本発明の有機ＥＬパネル（Ｐ）の構成で、絶縁層（１２）を有する一例を示す概略断面図（実施形態２）である。 FIG. 3 is a schematic sectional view (embodiment 2) showing an example having an insulating layer (12) in the configuration of the organic EL panel (P) of the present invention.
　基本的な構成は、図２で説明した実施形態１の構成と同様であり、陽極（３）とセパレーター（８）との間に、絶縁層（１２）を有している。このように絶縁層（１２）を設けることにより、同一発光エリア内での陽極と陰極間の絶縁性を更に高めることができ、短絡等を防止することができ、高い発光安定性を実現することができる。 The basic configuration is the same as that of the first embodiment described with reference to FIG. 2, and an insulating layer (12) is provided between the anode (3) and the separator (8). By providing the insulating layer (12) in this way, the insulation between the anode and the cathode in the same light emitting area can be further enhanced, a short circuit or the like can be prevented, and high light emission stability can be realized. Can do.
　（絶縁層）
　絶縁層は、陽極（３）の端部を覆うように形成されていることが好ましい。陽極の端部では有機機能層ユニット（Ｕ）の厚みが薄くなるため、絶縁層を形成することでショートし難くすることができる。絶縁層が形成された部分は、発光に寄与しない非発光領域とすることができる。 (Insulating layer)
The insulating layer is preferably formed so as to cover the end of the anode (3). Since the thickness of the organic functional layer unit (U) is reduced at the end of the anode, short-circuiting can be made difficult by forming an insulating layer. The portion where the insulating layer is formed can be a non-light emitting region that does not contribute to light emission.
　絶縁層の形成位置としては、発光エリア内で陽極が露出するように、絶縁層が形成されていればよい。発光領域の大きさとしては、特に限定されるものではなく、有機ＥＬパネルの用途等に応じて適宜設定される。 The insulating layer may be formed as long as the insulating layer is formed so that the anode is exposed in the light emitting area. The size of the light emitting region is not particularly limited, and is appropriately set according to the use of the organic EL panel.
　絶縁層の形成材料としては、感光性ポリイミド樹脂、アクリル系樹脂等の光硬化型樹脂、または熱硬化型樹脂、および無機材料等を挙げることができる。 Examples of the material for forming the insulating layer include photo-curing resins such as photosensitive polyimide resins and acrylic resins, thermosetting resins, and inorganic materials.
　絶縁層の形成方法としては、フォトリソグラフィー法、印刷法等の一般的な方法を用いることができるが、特に、フォトリソグラフィー法で形成することが好ましい。 As a method for forming the insulating layer, a general method such as a photolithography method or a printing method can be used, but it is particularly preferable to form the insulating layer by a photolithography method.
　〔実施形態３：基材にガスバリアー層を形成〕
　本発明においては、基材としてフレキシブル性樹脂基材を用い、かつフレキシブル性樹脂基材上にガスバリアー層を有している構成であることが好ましい形態である（実施形態３）。 [Embodiment 3: Forming a gas barrier layer on a substrate]
In this invention, it is a preferable form that it is the structure which uses a flexible resin base material as a base material and has a gas barrier layer on a flexible resin base material (Embodiment 3).
　図４で示す有機ＥＬパネル（Ｐ）は、基材上にガスバリアー層（２）を有する構成の一例を示す概略断面図（実施形態３）である。 The organic EL panel (P) shown in FIG. 4 is a schematic cross-sectional view (Embodiment 3) showing an example of a configuration having a gas barrier layer (2) on a substrate.
　基本的な構成は、上記実施態様２の図３で説明した構成と同一であるが、基材（１）と陽極（３）との間に、ガスバリアー層（２）を形成した構成である。 The basic configuration is the same as the configuration described in FIG. 3 of the second embodiment, except that a gas barrier layer (2) is formed between the base material (1) and the anode (3). .
　このようなガスバリアー層（２）を設けることにより、基材としてガラス基材に比べ、水蒸気透過度等が高いフレキシブル性樹脂基材に対し、高次のガスバリアー性を付与することができる。 By providing such a gas barrier layer (2), a higher-order gas barrier property can be imparted to a flexible resin substrate having a higher water vapor permeability and the like as a substrate than a glass substrate.
　〈ガスバリアー層〉
　基材（１）の片面又は両面で、少なくとも陽極（３、第１電極）が形成される側の全面に、光透過性のあるガスバリアー層（２）を形成することにより、水分や酸素など、有機ＥＬ素子の構成材料に対し劣化をもたらすものの浸入を抑制することができる。 <Gas barrier layer>
By forming a gas permeable gas barrier layer (2) on at least one side or both sides of the substrate (1) on the side where the anode (3, first electrode) is formed, moisture, oxygen, etc. Intrusion of materials that cause deterioration of the constituent materials of the organic EL element can be suppressed.
　ガスバリアー層（２）は、無機材料被膜だけでなく、有機材料との複合材料からなる被膜又はこれらの被膜を積層したハイブリッド被膜であってもよい。ガスバリアー層（２）の性能としては、ＪＩＳ（日本工業規格）－Ｋ７１２９（２００８年）に準拠した方法で測定した水蒸気透過度（環境条件：２５±０．５℃、相対湿度：９０±２％）が約０．０１ｇ／ｍ２・２４ｈ以下であり、ＪＩＳ－Ｋ７１２６（２００６年）に準拠した方法で測定した酸素透過度が約０．０１ｍｌ／ｍ２・２４ｈ・ａｔｍ以下、抵抗率が１×１０１２Ω・ｃｍ以上、光線透過率は可視光領域で約８０％以上であるような、ガスバリアー性を有する光透過性の絶縁膜であることが好ましい。 The gas barrier layer (2) may be not only an inorganic material film but also a film made of a composite material with an organic material or a hybrid film obtained by laminating these films. As the performance of the gas barrier layer (2), water vapor permeability measured by a method in accordance with JIS (Japanese Industrial Standard) -K7129 (2008) (environmental condition: 25 ± 0.5 ° C., relative humidity: 90 ± 2) %) Is about 0.01 g / m 2 · 24 h or less, the oxygen permeability measured by a method according to JIS-K7126 (2006) is about 0.01 ml / m 2 · 24 h · atm or less, and the resistivity is It is preferably a light-transmitting insulating film having gas barrier properties such that 1 × 10 12 Ω · cm or more and light transmittance is about 80% or more in the visible light region.
　ガスバリアー層（２）の形成材料としては、有機ＥＬ素子の劣化を招く、例えば水や酸素等のガスの有機ＥＬ素子への浸入を抑制できる材料であれば、任意の材料を用いることができる。 As a material for forming the gas barrier layer (2), any material can be used as long as it can suppress the intrusion of a gas such as water or oxygen into the organic EL element, which causes deterioration of the organic EL element. .
　ガスバリアー層（２）は、例えば、酸化ケイ素、窒化ケイ素、酸窒化ケイ素、炭化ケイ素、酸炭化ケイ素、酸化アルミニウム、窒化アルミニウム、酸化チタン、酸化ジルコニウム、酸化ニオブ、酸化モリブデン等の無機材料からなる被膜で構成することができ、好ましくは、窒化ケイ素や酸化ケイ素等のケイ素化合物を主原料とする構成である。 The gas barrier layer (2) is made of an inorganic material such as silicon oxide, silicon nitride, silicon oxynitride, silicon carbide, silicon oxycarbide, aluminum oxide, aluminum nitride, titanium oxide, zirconium oxide, niobium oxide, and molybdenum oxide. It can be comprised with a film, Preferably, it is the structure which uses silicon compounds, such as a silicon nitride and a silicon oxide, as a main raw material.
　ガスバリアー層の形成方法としては、従来公知の薄膜形成方法を適宜選択して用いることができ、例えば、真空蒸着法、スパッタ法、マグネトロンスパッタ法、分子線エピタキシー法、クラスターイオンビーム法、イオンプレーティング法、プラズマ重合法、大気圧プラズマ重合法（特開２００４－６８１４３号公報参照）、プラズマＣＶＤ（Ｃｈｅｍｉｃａｌ　Ｖａｐｏｒ　Ｄｅｐｏｓｉｔｉｏｎ）法、レーザーＣＶＤ法、熱ＣＶＤ法、ＡＬＤ（原子層堆積）法、また、ポリシラザン等を用いた湿式塗布法を適用することもできる。 As a method for forming the gas barrier layer, a conventionally known thin film forming method can be appropriately selected and used. For example, a vacuum deposition method, a sputtering method, a magnetron sputtering method, a molecular beam epitaxy method, a cluster ion beam method, an ion plate method can be used. Coating method, plasma polymerization method, atmospheric pressure plasma polymerization method (see JP 2004-68143 A), plasma CVD (Chemical Vapor Deposition) method, laser CVD method, thermal CVD method, ALD (atomic layer deposition) method, A wet coating method using polysilazane or the like can also be applied.
　〔実施形態４：有機ＥＬ素子の配置パターン〕
　複数の独立している発光エリア（有機ＥＬ素子）を有する本発明の有機ＥＬパネルにおいては、複数の発光エリアが、ストライプ状に並列配置されているパターンであることが好ましい形態である。 [Embodiment 4: Arrangement pattern of organic EL elements]
In the organic EL panel of the present invention having a plurality of independent light-emitting areas (organic EL elements), it is preferable that the plurality of light-emitting areas have a pattern arranged in parallel in a stripe shape.
　図５は、複数の発光エリアをストライプ状に配置した有機ＥＬパネルの一例を示す上面図及び概略断面図（実施形態４）である。 FIG. 5 is a top view and a schematic cross-sectional view (embodiment 4) showing an example of an organic EL panel in which a plurality of light emitting areas are arranged in a stripe shape.
　図５の（ａ）に示す構成では、広い面積からなる基材（１）上に、短冊状の有機ＥＬ素子（ＯＬＥＤ）より構成される発光エリアをストライプ状に配列した例を示してある。図５の（ａ）では、有機ＥＬ素子（ＯＬＥＤ）としては、ＯＬＥＤ１～ＯＬＥＤｎまでのｎ個を並列配置している。同一平面上にＯＬＥＤをストライプ状に配置する場合、そのＯＬＥＤの配置数としては、基材の大きさや、ＯＬＥＤの大きさにより、一概に規定することはできないが、最小構成は２つのＯＬＥＤを用いた構成であるが、本願発明の輝度均一性を達成する観点からは、好ましくは２～２０個の範囲内であり、さらに好ましくは２～１０個の範囲内である。したがって、一例としては、基材の幅が１０ｃｍ×１０ｃｍの大面積の有機ＥＬパネルにおいては、ＯＬＥＤによる発光エリアのサイズとしては、幅０．５ｃｍ×長さ１０ｃｍ～巾５ｃｍ×長さ１０ｃｍ、好ましくは巾１．０ｃｍ×長さ１０ｃｍ～巾５ｃｍ×長さ１０ｃｍの範囲内となるが、これらの発光エリア面積は、基材のサイズ及びＯＬＥＤの配置数により、適宜選択することができる。 The configuration shown in FIG. 5A shows an example in which light emitting areas composed of strip-shaped organic EL elements (OLEDs) are arranged in stripes on a substrate (1) having a large area. In FIG. 5A, n organic EL elements (OLEDs) from OLED 1 to OLED n are arranged in parallel. When OLEDs are arranged in stripes on the same plane, the number of OLEDs to be arranged cannot be unconditionally defined by the size of the substrate or the size of the OLEDs, but the minimum configuration uses two OLEDs. However, from the viewpoint of achieving the luminance uniformity of the present invention, it is preferably in the range of 2 to 20, more preferably in the range of 2 to 10. Therefore, as an example, in a large area organic EL panel having a substrate width of 10 cm × 10 cm, the size of the light emitting area by OLED is 0.5 cm wide × 10 cm long × 5 cm wide × 10 cm long, preferably Is within the range of width 1.0 cm × length 10 cm to width 5 cm × length 10 cm. The area of the light emitting area can be appropriately selected depending on the size of the substrate and the number of OLEDs arranged.
　また、図５で示す「非発光エリア」の幅としては、おおむね０．２～１．０ｍｍの範囲内であることが好ましい。 Further, the width of the “non-light emitting area” shown in FIG. 5 is preferably within a range of about 0.2 to 1.0 mm.
　図５の（ｂ）は、図５の（ａ）で示した構成の有機ＥＬパネル（Ｐ）の概略断面図であり、ＯＬＥＤ１～ＯＬＥＤｎまでのｎ個のＯＬＥＤが並列配置している有機ＥＬ素子（ＯＬＥＤ）群において、分割されている一方の発光エリアを構成する陽極（３）の端部と、隣接する他方の発光エリアを構成する陰極（７）の端部とが直列に電気的に接続されている。更に、一方の端部に配置されているＯＬＥＤ（例えば、図５の（ｂ）で示す左端部のＯＬＥＤ１）の陽極（３）と、他方の端部に配置されているＯＬＥＤ（例えば、図５の（ｂ）で示す右端部のＯＬＥＤｎ）の陰極（７）間が、配線（１８）により接続され、その回路内に印加電源（１３）が設けられており、各ＯＬＥＤを発光させるための電力供給を行う。 FIG. 5B is a schematic cross-sectional view of the organic EL panel (P) having the configuration shown in FIG. 5A, in which n OLEDs from OLED 1 to OLED n are arranged in parallel. In the EL element (OLED) group, the end of the anode (3) constituting one divided light emitting area and the end of the cathode (7) constituting the other adjacent light emitting area are electrically connected in series. It is connected to the. Furthermore, the anode (3) of the OLED disposed at one end (for example, the leftmost OLED 1 shown in FIG. 5B) and the OLED disposed at the other end (for example, FIG. 5 (b), the cathode (7) of OLED n ) at the right end is connected by a wiring (18), and an applied power source (13) is provided in the circuit so that each OLED emits light. Power supply.
　〔有機ＥＬパネルの概略回路図〕
　図６Ａに従来型の有機ＥＬパネルの回路図を示し、図６Ｂには本発明の有機ＥＬパネルの回路図を示す。 [Schematic circuit diagram of organic EL panel]
FIG. 6A shows a circuit diagram of a conventional organic EL panel, and FIG. 6B shows a circuit diagram of the organic EL panel of the present invention.
　図６Ａは、従来型の有機ＥＬパネル（Ｐ）の回路図であり、単一の大型の有機ＥＬ素子（ＯＬＥＤ）で構成した際の回路図で、印加電源（１３）より、有機ＥＬ素子に電圧Ｖ、電流Ｉを印加して発光させるが、この構成では、広い面積のＯＬＥＤに大容量の電流Ｉが流れるため、有機ＥＬ素子面内で、電流が多く流れる領域と少なくしか流れない領域が発生し、輝度ムラが発生しやすくなる。有機ＥＬ素子の輝度は、流れる電流が大きくなればなるほど高くなるため、このような電流差が発生することにより、輝度ムラが発生しやすい状態にあった。 FIG. 6A is a circuit diagram of a conventional organic EL panel (P), and is a circuit diagram when configured with a single large organic EL element (OLED). A voltage V and a current I are applied to cause light emission. In this configuration, a large-capacity current I flows through a large area OLED. Occur, and uneven brightness tends to occur. Since the luminance of the organic EL element becomes higher as the flowing current increases, the occurrence of such a current difference tends to cause uneven luminance.
　これに対し、図６Ｂに示す回路図では、複数のＯＬＥＤ（ＯＬＥＤ１～ＯＬＥＤｎ）を並列配置した本発明の有機ＥＬパネル（Ｐ）においては、有機ＥＬ素子に印加電源（１３）より電圧Ｎ×Ｖ、電流Ｉを印加して発光させるが、個々の有機ＥＬ素子（ＯＬＥＤ）に流れる電流は、Ｉ／Ｎとなり、有機ＥＬ素子間における電流差が生じ難くなるため、輝度ムラが発生しにくくなるため、発光均一性に優れた大型の有機ＥＬパネルを実現することができる。 In contrast, in the circuit diagram shown in FIG. 6B, in the organic EL panel (P) of the present invention in which a plurality of OLEDs (OLED 1 to OLED n ) are arranged in parallel, the voltage N is applied to the organic EL element from the applied power supply (13). × V, current I is applied to cause light emission, but the current flowing through each organic EL element (OLED) is I / N, and it is difficult for current differences between the organic EL elements to occur, so luminance unevenness is unlikely to occur. Therefore, it is possible to realize a large-sized organic EL panel having excellent light emission uniformity.
　〔実施形態５：封止部材を具備した有機ＥＬ素子〕
　図７は、本発明の有機ＥＬパネルの構成で、封止部材を設けた構成の一例を示す概略断面図（実施形態５）である。 [Embodiment 5: Organic EL device provided with sealing member]
FIG. 7: is a schematic sectional drawing (embodiment 5) which shows an example of the structure which provided the sealing member by the structure of the organic electroluminescent panel of this invention.
　図７に示す有機ＥＬパネル（Ｐ）では、上記説明した図４で示した陰極まで形成した複数の有機ＥＬ素子（ＯＬＥＤ）を具備した有機ＥＬパネル（Ｐ）に対し、更にその上部に封止部材を形成している一例を示してある。 In the organic EL panel (P) shown in FIG. 7, the organic EL panel (P) having a plurality of organic EL elements (OLED) formed up to the cathode shown in FIG. An example of forming a member is shown.
　図７で示すように、複数の有機ＥＬ素子（ＯＬＥＤ）の全面に、封止用接着剤（９）を付与した後、最表面にガスバリアー層（１０）を具備している封止部材（１１）を形成する。 As shown in FIG. 7, after providing the sealing adhesive (9) to the whole surface of a plurality of organic EL elements (OLED), a sealing member having a gas barrier layer (10) on the outermost surface ( 11).
　封止部材としては、有機ＥＬ素子の表示領域を覆うように配置されていればよく、凹板状でも、平板状でもよい。また透明性を有していれば電気絶縁性は特に限定されない。 The sealing member may be disposed so as to cover the display area of the organic EL element, and may be concave or flat. Moreover, if it has transparency, electrical insulation will not be specifically limited.
　具体的には、フレキシブル性を備えた光透過性のガラス基板、樹脂基板、フィルム、金属フィルム（金属箔）等が挙げられる。ガラス基板としては、特にソーダ石灰ガラス、バリウム・ストロンチウム含有ガラス、鉛ガラス、アルミノケイ酸ガラス、ホウケイ酸ガラス、バリウムホウケイ酸ガラス、石英等を挙げることができる。また、樹脂基板としては、ポリカーボネート、アクリル、ポリエチレンテレフタレート、ポリエーテルサルファイド、ポリサルフォン等を挙げることができる。 Specifically, a light transmissive glass substrate, a resin substrate, a film, a metal film (metal foil) having flexibility, and the like can be given. Examples of the glass substrate include soda-lime glass, barium / strontium-containing glass, lead glass, aluminosilicate glass, borosilicate glass, barium borosilicate glass, and quartz. Examples of the resin substrate include polycarbonate, acrylic, polyethylene terephthalate, polyether sulfide, and polysulfone.
　封止用接着剤としては、ポリウレタン系、ポリエステル系、エポキシ系、アクリル系等の接着剤を用いることができる。必要に応じて硬化剤を併用してもよい。ホットメルトラミネーション法やエクストルージョンラミネート法および共押出しラミネーション法も使用できるがドライラミネート方式が好ましい。 As the sealing adhesive, polyurethane-based, polyester-based, epoxy-based, acrylic-based adhesives can be used. You may use a hardening | curing agent together as needed. A hot melt lamination method, an extrusion lamination method and a coextrusion lamination method can also be used, but a dry lamination method is preferred.
　本発明においては、封止部材としては、有機ＥＬ素子を薄膜化することできる観点から、樹脂基板及びカラス基板を好ましく使用することができる。さらに、樹脂基板は、ＪＩＳ　Ｋ　７１２９－１９９２に準拠した方法で測定された温度２５±０．５℃、相対湿度９０±２％ＲＨにおける水蒸気透過度が、１×１０－３ｇ／ｍ２・２４ｈ以下であることが好ましく、さらには、ＪＩＳ　Ｋ　７１２６－１９８７に準拠した方法で測定された酸素透過度が、１×１０－３ｍｌ／ｍ２・２４ｈ・ａｔｍ（１ａｔｍは、１．０１３２５×１０５Ｐａである）以下であって、温度２５±０．５℃、相対湿度９０±２％ＲＨにおける水蒸気透過度が、１×１０－３ｇ／ｍ２・２４ｈ以下であることが好ましい。この条件を満たすため、前述の基材にて説明したのと同様のガスバリアー層を設けることが好ましい形態である。 In the present invention, as the sealing member, a resin substrate and a crow substrate can be preferably used from the viewpoint of reducing the thickness of the organic EL element. Further, the resin substrate has a water vapor transmission rate of 1 × 10 −3 g / m 2 .multidot.m at a temperature of 25 ± 0.5 ° C. and a relative humidity of 90 ± 2% RH measured by a method according to JIS K 7129-1992. The oxygen permeability measured by a method according to JIS K 7126-1987 is preferably 1 × 10 −3 ml / m 2 · 24 h · atm (1 atm is 1.01325 × 10 5 a Pa) equal to or lower than a temperature of 25 ± 0.5 ° C., water vapor permeability at a relative humidity of 90 ± 2% RH is preferably not more than 1 × 10 -3 g / m 2 · 24h. In order to satisfy this condition, it is a preferable embodiment to provide a gas barrier layer similar to that described for the base material.
　封止部材と有機ＥＬ素子の表示領域（発光領域）との間隙には、気相及び液相では窒素、アルゴン等の不活性気体やフッ化炭化水素、シリコンオイルのような不活性液体を注入することもできる。また、封止部材と有機ＥＬ素子の表示領域との間隙を真空とすることや、間隙に吸湿性化合物を封入することもできる。 In the gap between the sealing member and the display area (light emitting area) of the organic EL element, an inert gas such as nitrogen or argon, or an inert liquid such as fluorocarbon or silicon oil is injected in the gas phase and liquid phase. You can also Further, the gap between the sealing member and the display area of the organic EL element can be evacuated, or a hygroscopic compound can be sealed in the gap.
　〔有機ＥＬ素パネルの製造方法：実施形態６〕
　次いで、本発明の有機ＥＬパネルの製造方法の概略について説明する。 [Method for Manufacturing Organic EL Panel: Embodiment 6]
Next, an outline of a method for producing the organic EL panel of the present invention will be described.
　本発明の有機Ｅパネルの製造方法は、上記説明した構成からなる非発光時の波長５５０ｎｍにおける光透過率が５０％以上である有機エレクトロルミネッセンス素子を具備した有機ＥＬパネルの製造方法であり、当該有機エレクトロルミネッセンス素子において、基材上に、少なくとも陽極、有機機能層ユニット及び陰極より構成される発光エリアを、複数に分割して形成し、前記陰極を、前記陽極上に設けたセパレーターにより分離したパターンを形成し、分割されている一方の発光エリアを構成する陽極を、隣接する他方の発光エリアを構成する陰極と、直列に電気的に接続し、かつ、前記陽極、陰極及びセパレーターを、フォトリソグラフィー法により形成することを特徴とする。 The method for producing an organic E panel of the present invention is a method for producing an organic EL panel having an organic electroluminescence element having a light transmittance of 50% or more at a wavelength of 550 nm when not emitting light having the above-described configuration, In the organic electroluminescence element, a light emitting area composed of at least an anode, an organic functional layer unit, and a cathode is formed on a substrate by dividing into a plurality of parts, and the cathode is separated by a separator provided on the anode. A pattern is formed, and the anode constituting one of the divided light emitting areas is electrically connected in series with the cathode constituting the other neighboring light emitting area, and the anode, cathode and separator are connected to the photo It is formed by a lithography method.
　加えて、陽極と前記セパレーターとの間に、フォトリソグラフィー法を用いて絶縁層を形成する製造方法が好ましい実施形態である。 In addition, a manufacturing method in which an insulating layer is formed between the anode and the separator using a photolithography method is a preferred embodiment.
　代表的な有機ＥＬパネル（Ｐ）の各構成部材の形成工程としては、基板（１）上に、真空蒸着法、スパッタ法、ＣＶＤ法、湿式塗布法によりガスバリアー層（２）を形成した後、陽極（３）、絶縁層（１２）、及びセパレーター（８）をフォトリソグラフィー法により成膜した後、有機機能層ユニット（Ｕ）及び陰極（７）を蒸着法により形成し、最後に、湿式塗布法等で、封止用接着剤（９）を形成した後、ガスバリアー層（１０）を有する封止基板（１１）で、全面を封止して、有機ＥＬパネル（Ｐ）を作製する。 As a process for forming each constituent member of a typical organic EL panel (P), a gas barrier layer (2) is formed on the substrate (1) by vacuum deposition, sputtering, CVD, or wet coating. The anode (3), the insulating layer (12), and the separator (8) are formed by photolithography, the organic functional layer unit (U) and the cathode (7) are formed by vapor deposition, and finally wet. After forming the sealing adhesive (9) by a coating method or the like, the entire surface is sealed with a sealing substrate (11) having a gas barrier layer (10) to produce an organic EL panel (P). .
　（フォトリソグラフィー法）
　本発明では、フォトリソグラフィー法を用いたエッチング加工（パターニング）により、所望のパターンの陽極（３）、絶縁層（１２）、及びセパレーター（８）を形成することができる。上記形成にフォトリソグラフィー法を適用することにより、高精度で精細な陽極（３）、絶縁層（１２）、及びセパレーター（８）を形成でき、極めて狭い非発光エリアを形成することができる。 (Photolithography method)
In the present invention, the anode (3), the insulating layer (12), and the separator (8) having a desired pattern can be formed by etching (patterning) using a photolithography method. By applying a photolithography method to the above formation, a highly accurate and fine anode (3), insulating layer (12), and separator (8) can be formed, and an extremely narrow non-light emitting area can be formed.
　本発明に適用可能なフォトリソグラフィー法とは、レジスト塗布、（予備加熱、）露光、現像、リンス、（前処理）、エッチング、レジスト剥離の各工程を経ることにより、陽極（３）、絶縁層（１２）及びセパレーター（８）を所望の高精細パターンで形成する方法である。本発明では、従来公知の一般的なフォトリソグラフィー法を適宜利用することができ、例えば、特開２０１０－１４５５３２号公報、特開２０１２－１１８４２５号公報、特開２０１３－２５４４７号公報、特開２０１３－２５４４８号公報等に記載されている方法を参考にすることができる。 The photolithographic method applicable to the present invention includes resist coating, (preheating), exposure, development, rinsing, (pretreatment), etching, and resist stripping, and then the anode (3), the insulating layer. This is a method for forming (12) and the separator (8) with a desired high-definition pattern. In the present invention, a conventionally known general photolithography method can be used as appropriate. For example, JP 2010-145532 A, JP 2012-118425 A, JP 2013-25447 A, JP 2013 2013 A. Reference can be made to the method described in Japanese Patent No. 25448.
　フォトリソグラフィー法としては、例えば、レジストとしてはポジ型又はネガ型のいずれのレジストでも使用可能である。また、レジスト塗布後、必要に応じて予備加熱又はプリベークを実施することができる。露光に際しては、所望のパターンを有するパターンマスクを配置し、その上から、用いたレジストに適合する波長の光、一般には紫外光を照射すればよい。露光後、用いたレジストに適合する現像液で現像を行うことができる。現像後、水等のリンス液で現像を止めるとともに洗浄を行うことで、レジストパターンが形成される。 As the photolithography method, for example, either a positive type resist or a negative type resist can be used. In addition, after applying the resist, preheating or prebaking can be performed as necessary. At the time of exposure, a pattern mask having a desired pattern may be disposed, and light having a wavelength suitable for the resist used, generally ultraviolet light may be irradiated thereon. After the exposure, development can be performed with a developer that is compatible with the resist used. After the development, the resist pattern is formed by stopping the development with a rinse solution such as water and washing.
　次いで、形成されたレジストパターンを、必要に応じて前処理又はポストベークを実施してから、エッチングで彫り込むことができる。エッチング後、残留するレジストを剥離することによって、所望のパターンを有する陽極（３）、絶縁層（１２）、及びセパレーター（８）が得られる。このように、本発明に適用されるフォトリソグラフィー法は、当業者に一般に認識されている方法であり、その具体的な適用態様は当業者であれば、目的に応じて容易に選定することができる。 Next, the formed resist pattern can be engraved by etching after pre-processing or post-baking as necessary. After etching, the remaining resist is peeled off to obtain an anode (3), an insulating layer (12), and a separator (8) having a desired pattern. As described above, the photolithography method applied to the present invention is a method generally recognized by those skilled in the art, and a specific application mode can be easily selected according to the purpose by those skilled in the art. it can.
　図８は、前記図７で示した実施形態５の有機ＥＬパネル（Ｐ）の作製手順の一例を示す工程フロー図（実施形態６）である。 FIG. 8 is a process flow diagram (Embodiment 6) showing an example of the manufacturing procedure of the organic EL panel (P) of Embodiment 5 shown in FIG.
　はじめに、図８の（ａ）で示すように、光透過性を有する基材（１）上にガスバリアー層（２）を形成する。ガスバリアー層（２）の形成方法としては、前述のとおり、真空蒸着法、スパッタ法、マグネトロンスパッタ法、分子線エピタキシー法、クラスターイオンビーム法、イオンプレーティング法、プラズマ重合法、大気圧プラズマ重合法、プラズマＣＶＤ法や、ポリシラザン等を用いた湿式塗布法を用いて形成する。 First, as shown in FIG. 8A, a gas barrier layer (2) is formed on a light-transmitting substrate (1). As described above, the gas barrier layer (2) can be formed by vacuum deposition, sputtering, magnetron sputtering, molecular beam epitaxy, cluster ion beam, ion plating, plasma polymerization, atmospheric pressure plasma It is formed by a wet coating method using a combination method, a plasma CVD method, polysilazane, or the like.
　次いで、図８の（ｂ）で示すように、ガスバリアー層（２）上の所定の位置に、フォトリソグラフィー法を用いて、複数の光透過性を有する陽極（３）をそれぞれ離間した状態で形成する。 Next, as shown in FIG. 8B, a plurality of light-transmitting anodes (3) are separated from each other at predetermined positions on the gas barrier layer (2) by using a photolithography method. Form.
　次いで、図８の（ｃ）で示すように、陽極上の特定のエリア（端部）に、絶縁層（１２）を、同じくフォトリソグラフィー法を用いて形成する。 Next, as shown in FIG. 8 (c), an insulating layer (12) is formed in a specific area (edge) on the anode by the same photolithography method.
　次いで、図８の（ｄ）で示すように、形成した絶縁層（１２）上に、セパレーター（８）を、同じくフォトリソグラフィー法を用いて形成する。 Next, as shown in FIG. 8D, a separator (8) is formed on the formed insulating layer (12) using the same photolithography method.
　次いで、図８の（ｅ）で示すように、例えば、キャリア輸送機能層群１（４、例えば、正孔注入層及び正孔輸送層等）、発光層（５）、キャリア輸送機能層群２（６、電子輸送層等）より構成される複数の有機機能層ユニット（Ｕ）を形成する。 Next, as shown in FIG. 8E, for example, the carrier transport function layer group 1 (4, for example, a hole injection layer and a hole transport layer), the light emitting layer (5), the carrier transport function layer group 2 A plurality of organic functional layer units (U) composed of (6, electron transport layer, etc.) are formed.
　これら有機機能層ユニットを形成している各層の形成は、スピンコート法、キャスト法、インクジェット法、蒸着法、印刷法等があるが、均質な層が得られやすく、かつ、高精度で成膜を行うことができる点で、ファインマスク（Ｍ）を用いた蒸着法を適用することが好ましい。具体的には、蒸着用の加熱ボートに各有機機能層ユニット形成用の各原料を充填し、加熱ボートを加熱して、ファインマスクを介して、光透過性を有する陽極（３）上に、有機機能層ユニット（Ｕ）の各層のパターンを形成する。 Each of the organic functional layer units can be formed by spin coating, casting, ink jet, vapor deposition, printing, etc., but it is easy to obtain a homogeneous layer and is formed with high accuracy. It is preferable to apply a vapor deposition method using a fine mask (M) in that it can be performed. Specifically, each raw material for forming each organic functional layer unit is filled in a heating boat for vapor deposition, the heating boat is heated, and on the anode (3) having light transmittance through a fine mask, A pattern of each layer of the organic functional layer unit (U) is formed.
　この時、有機機能層ユニット層（Ｕ）を構成する各層ごとに異なる形成法を適用しても良い。これらの各層の形成に蒸着法を採用する場合、その蒸着条件は使用する化合物の種類等により異なるが、一般にボート加熱温度を５０～４５０℃の範囲、真空度を１×１０－６～１×１０－２Ｐａの範囲、蒸着速度０．０１～５０ｎｍ／秒の範囲、基板温度－５０～３００℃の範囲、層厚０．１～５μｍの範囲内で、各条件を適宜選択することが望ましい。 At this time, a different forming method may be applied to each layer constituting the organic functional layer unit layer (U). When a vapor deposition method is employed for forming each of these layers, the vapor deposition conditions vary depending on the type of compound used, but generally the boat heating temperature is in the range of 50 to 450 ° C., and the degree of vacuum is 1 × 10 −6 to 1 ×. Each condition is preferably selected as appropriate within the range of 10 −2 Pa, the deposition rate of 0.01 to 50 nm / second, the substrate temperature of −50 to 300 ° C., and the layer thickness of 0.1 to 5 μm. .
　次いで、図８の（ｆ）で示すように、複数の有機機能層ユニット（Ｕ）上で、２つのセパレーター（８）により分離されている特定のエリア全面に、光透過性を有する陰極（７）を形成する。この時、隣接する位置形成してある一方の有機ＥＬ素子の陽極（３）の端部と、導電性接着剤等を介して電気的に接続させるように形成する。具体的には、蒸着用の加熱ボートに陰極形成用の原料を充填し、当該加熱ボートを加熱して、ファインマスクを介して、有機機能層ユニット（Ｕ）上及び隣接する陽極（３）上に、陰極（７）を形成する。この時、陰極（７）と、隣接する陽極（３）間は、導電性接着剤（不図示）により電気的接続されている。 Next, as shown in FIG. 8 (f), a light-transmitting cathode (7) is formed on the entire surface of a specific area separated by two separators (8) on the plurality of organic functional layer units (U). ). At this time, it is formed so as to be electrically connected to the end portion of the anode (3) of one organic EL element formed at an adjacent position via a conductive adhesive or the like. Specifically, a cathode forming raw material is filled in a vapor deposition heating boat, the heating boat is heated, and the organic functional layer unit (U) and the adjacent anode (3) are passed through a fine mask. Next, a cathode (7) is formed. At this time, the cathode (7) and the adjacent anode (3) are electrically connected by a conductive adhesive (not shown).
　次いで、図８の（ｇ）で示すように、陰極（７）を形成した後、これら光透過性を有する基材（１）、ガスバリアー層（２）、陽極（３）、絶縁層（１２）、セパレーター（８）、有機機能層ユニット（Ｕ）及び陰極（７）の全面を、封止用樹脂層（９）と、ガスバリアー層（１０）を有する封止部材（１１）で封止する。 Next, as shown in FIG. 8 (g), after forming the cathode (7), the light-transmitting substrate (1), gas barrier layer (2), anode (3), insulating layer (12) ), The entire surface of the separator (8), the organic functional layer unit (U) and the cathode (7) is sealed with a sealing member (11) having a sealing resin layer (9) and a gas barrier layer (10). To do.
　〔実施形態７：陰極を薄膜銀層で形成〕
　本発明においては、光透過性を有する陰極が、含窒素化合物を用いて構成された下地層と、当該下地層上に、銀又は銀を主成分とした合金で構成されている薄膜銀層（陰極）を有する構成であることが好ましい形態の一つである。 [Embodiment 7: Forming the cathode as a thin film silver layer]
In the present invention, a light-transmitting cathode is an underlayer composed of a nitrogen-containing compound, and a thin-film silver layer composed of silver or an alloy containing silver as a main component on the underlayer ( One of the preferred embodiments is a structure having a cathode.
　図９は、陰極として、下地層（１４）とその上に、銀又は銀を主成分とした合金で構成されている薄膜銀層（１５）を設けた構成を示してある。 FIG. 9 shows a structure in which a base layer (14) and a thin film silver layer (15) made of silver or an alloy containing silver as a main component are provided thereon as a cathode.
　上記図９で記載した構成とすることにより、下地層上に銀又は銀を主成分とした合金で構成されている陰極を形成する際には、陰極を構成する銀原子が、下地層に含有されている窒素原子を有する化合物と相互作用を生じることにより、該下地層表面上での銀原子の拡散距離が減少し、特定箇所での銀原子の凝集を抑えることができ、均質な薄膜銀層（１５）を得ることができる。 With the configuration described in FIG. 9 above, when forming a cathode composed of silver or an alloy containing silver as a main component on the underlayer, silver atoms constituting the cathode are contained in the underlayer. By producing an interaction with a compound having a nitrogen atom, the diffusion distance of silver atoms on the surface of the underlayer is reduced, so that aggregation of silver atoms at a specific location can be suppressed, and a homogeneous thin film silver A layer (15) can be obtained.
　すなわち、銀原子は、まず窒素原子を有する化合物、更に詳しくは、銀原子と親和性のある芳香族性に関与しない非共有電子対を持つ窒素原子を有する非対称性化合物を含有する下地層表面上で２次元的な核を形成し，それを中心に２次元の単結晶層を形成するという単層成長型（Ｆｒａｎｋ－ｖａｎ　ｄｅｒ　Ｍｅｒｗｅ：ＦＭ型）の膜成長によって成膜されるようになり、均質性の高い薄膜の銀膜を形成することができる。 That is, the silver atom is first a compound having a nitrogen atom, and more specifically, on the surface of the underlayer containing an asymmetric compound having a nitrogen atom having an unshared electron pair that does not participate in aromaticity having an affinity for the silver atom. The film is formed by single-layer growth type (Frank-van der Merwe: FM type) film formation in which a two-dimensional nucleus is formed at the center and a two-dimensional single crystal layer is formed around the two-dimensional nucleus. A thin silver film with high homogeneity can be formed.
　（下地層）
　下地層を構成する材料としては、特に限定されるものではなく、その上に形成する陰極の構成材料である銀の凝集を抑制できるものであり、窒素原子を含んだ化合物等が挙げられる。 (Underlayer)
The material constituting the underlayer is not particularly limited, and can suppress aggregation of silver, which is a constituent material of the cathode formed thereon, and includes compounds containing nitrogen atoms.
　下地層（１４）を構成するのに用いることができる窒素原子含有化合物としては、分子内に窒素原子を含んでいる化合物であれば、特に限定はないが、窒素原子をヘテロ原子とした複素環を有する化合物が好ましい。窒素原子をヘテロ原子とした複素環としては、アジリジン、アジリン、アゼチジン、アゼト、アゾリジン、アゾール、アジナン、ピリジン、アゼパン、アゼピン、イミダゾール、ピラゾール、オキサゾール、チアゾール、イミダゾリン、ピラジン、モルホリン、チアジン、インドール、イソインドール、ベンゾイミダゾール、プリン、キノリン、イソキノリン、キノキサリン、シンノリン、プテリジン、アクリジン、カルバゾール、ベンゾ－Ｃ－シンノリン、ポルフィリン、クロリン及びコリン等が挙げられる。 The nitrogen atom-containing compound that can be used to form the underlayer (14) is not particularly limited as long as it is a compound containing a nitrogen atom in the molecule, but a heterocycle having a nitrogen atom as a heteroatom. A compound having is preferred. Examples of the heterocycle having a nitrogen atom as a hetero atom include aziridine, azirine, azetidine, azeto, azolidine, azole, azinane, pyridine, azepan, azepine, imidazole, pyrazole, oxazole, thiazole, imidazoline, pyrazine, morpholine, thiazine, indole, Examples include isoindole, benzimidazole, purine, quinoline, isoquinoline, quinoxaline, cinnoline, pteridine, acridine, carbazole, benzo-C-cinnoline, porphyrin, chlorin and choline.
　さらには、下地層（１４）が含有する窒素原子含有化合物は、芳香族性に関与しない非共有電子対を持つ窒素原子を有する芳香族複素環化合物であることが好ましい。 Furthermore, the nitrogen atom-containing compound contained in the underlayer (14) is preferably an aromatic heterocyclic compound having a nitrogen atom having an unshared electron pair not involved in aromaticity.
　これらの窒素原子含有化合物の具体例としては、特開２０１５－０４６３６４号公報の段落（００９７）～同（０２２１）に記載の例示化合物Ｎｏ．１～Ｎｏ．１３４を挙げることができる。 Specific examples of these nitrogen atom-containing compounds include Exemplified Compound Nos. Described in paragraphs (0097) to (0221) of JP-A-2015-046364. 1-No. 134.
　〔実施形態８：光学調整層の形成〕
　本発明においては、陰極の上部に光学調整層を設ける構成が好ましい形態である。 [Embodiment 8: Formation of optical adjustment layer]
In the present invention, a configuration in which an optical adjustment layer is provided on the cathode is a preferred embodiment.
　図１０は、本発明に適用可能な有機ＥＬ素子の構成の一例で、上記図９で説明した構成の薄膜銀層（１５）の上部に、光学調整層（１６）を形成した構成を示す概略断面図（実施形態６）である。 FIG. 10 is an example of a configuration of an organic EL element applicable to the present invention, and schematically shows a configuration in which an optical adjustment layer (16) is formed on the thin film silver layer (15) having the configuration described in FIG. It is sectional drawing (Embodiment 6).
　本発明に適用可能な光学調整層とは、光学干渉作用により光透過性材料の透過率を向上させる役割を果たすものをいう。 The optical adjustment layer applicable to the present invention means a layer that plays a role of improving the transmittance of the light transmissive material by the optical interference action.
　本発明に適用可能な光学調整層を構成する材料としては、適当な屈折率が得られれば特に制限なく既存の化合物を利用できる。有機ＥＬの陰極上に、ダメージなく成膜できるという点から、真空蒸着法を適用できる化合物が好ましい。 As a material constituting the optical adjustment layer applicable to the present invention, an existing compound can be used without particular limitation as long as an appropriate refractive index is obtained. A compound to which a vacuum deposition method can be applied is preferable from the viewpoint that a film can be formed on the organic EL cathode without damage.
　光学調整層の形成材料としては、例えば、Ａｌ２Ｏ３（屈折率１．６）、ＣｅＯ３（屈折率２．２）、Ｇａ２Ｏ３（屈折率１．５）、ＨｆＯ２（屈折率２．０）、ＩＴＯ（インジウム・スズ酸化物　屈折率２．１）、ＩＺＯ（インジウム・亜鉛酸化物、屈折率２．１）、ＭｇＯ（屈折率１．７）、Ｎｂ２Ｏ５（屈折率２．３）、ＳｉＯ２（屈折率１．５）、Ｔａ２Ｏ５（屈折率２．２）、ＴｉＯ２（屈折率２．３～２．５）、Ｙ２Ｏ３（屈折率１．９）、ＺｎＯ（屈折率２．１）、ＺｒＯ２（屈折率２．１）、ＡｌＦ３（１．４）、ＣａＦ２（１．２～１．４）、ＣｅＦ３（１．６）、ＧｄＦ３（１．６）、ＬａＦ３（１．５９）、ＬｉＦ（１．３）、ＭｇＦ２（１．４）、ＮａＦ（１．３）等を用いることができる。 As a material for forming the optical adjustment layer, for example, Al 2 O 3 (refractive index 1.6), CeO 3 (refractive index 2.2), Ga 2 O 3 (refractive index 1.5), HfO 2 (refractive index). 2.0), ITO (indium tin oxide, refractive index 2.1), IZO (indium zinc oxide, refractive index 2.1), MgO (refractive index 1.7), Nb 2 O 5 (refractive index). 2.3), SiO 2 (refractive index 1.5), Ta 2 O 5 (refractive index 2.2), TiO 2 (refractive index 2.3 to 2.5), Y 2 O 3 (refractive index 1. 9), ZnO (refractive index 2.1), ZrO 2 (refractive index 2.1), AlF 3 (1.4), CaF 2 (1.2 to 1.4), CeF 3 (1.6), GdF 3 (1.6), LaF 3 (1.59), LiF (1.3), MgF 2 (1.4), NaF (1.3), etc. can be used. wear.
　〔実施形態９：電気接続ユニット（ＦＰＣ）の適用〕
　本発明においては、有機ＥＬパネルと外部電極との接続部が、導電性接着剤により電気的接続されている構成であることが好ましく、更には外部電極が、光透過性を有するフレキシブルプリント回路（ＦＰＣ）より構成されることが好ましい形態である。 [Embodiment 9: Application of Electrical Connection Unit (FPC)]
In this invention, it is preferable that the connection part of an organic electroluminescent panel and an external electrode is the structure electrically connected by the electroconductive adhesive, and also the external electrode is a flexible printed circuit (with light transmittance) ( FPC) is a preferred form.
　図１１は、本発明に適用可能な有機ＥＬパネルと外部電極との電気的接続方法の一例を示す概略図である。 FIG. 11 is a schematic diagram showing an example of an electrical connection method between an organic EL panel and external electrodes applicable to the present invention.
　図１１においては、複数の有機ＥＬ素子（ＯＬＥＤ）を並列配置してある有機ＥＬパネル（Ｐ）の両端部設けた引出電極（１７）に対し、外部電極として光透過性を有するフレキシブルプリント回路（ＦＰＣ、２０）を、異方性導電膜（ＡＣＦ、１９）を介して接続している一例を示している。 In FIG. 11, a flexible printed circuit having optical transparency as an external electrode with respect to the extraction electrode (17) provided at both ends of the organic EL panel (P) in which a plurality of organic EL elements (OLED) are arranged in parallel. An example in which the FPC, 20) is connected via an anisotropic conductive film (ACF, 19) is shown.
　本発明の有機ＥＬパネルの形成においては、電気接続ユニットとして、透過性の高いＦＰＣ（フレキシブルプリント回路）を適用することができる。ＦＰＣ（Ｆｌｅｘｉｂｌｅ　ｐｒｉｎｔｅｄ　ｃｉｒｃｕｉｔｓ）とは、「フレキシブルプリント回路基板」や「フレキシブルプリント配線板」とも呼ばれ、絶縁性を持った薄く柔らかいベースフィルム（ポリイミド等）と銅箔等の導電性金属を貼り合わせた基材に電気回路を形成した基板をいう。 In the formation of the organic EL panel of the present invention, a highly transmissive FPC (flexible printed circuit) can be applied as the electrical connection unit. FPC (Flexible printed circuits) is also called "flexible printed circuit board" or "flexible printed wiring board", and a thin and soft base film (polyimide, etc.) with insulation is bonded to a conductive metal such as copper foil. A substrate in which an electric circuit is formed on a substrate.
　電気接続ユニットであるＦＰＣは、フレキシブル基板の表面側に回路部を有し、裏面側には配線を有している。 FPC which is an electrical connection unit has a circuit part on the front side of the flexible substrate and wiring on the back side.
　電気接続ユニット（ＦＰＣ）を構成するフレキシブル基板としては、透明でフレキシブル性を有し、かつ十分な機械的強度を備えたプラスチック材料であれば特に制限はなく、ポリイミド樹脂（ＰＩ）、ポリカーボネート樹脂、ポリエチレンテレフタレート樹脂（ＰＥＴ）、ポリエチレンナフタレート樹脂（ＰＥＮ）、シクロオレフィン樹脂（ＣＯＰ）等が挙げられるが、好ましくは、ポリイミド樹脂（ＰＩ）、ポリエチレンテレフタレート樹脂（ＰＥＴ）、ポリエチレンナフタレート樹脂（ＰＥＮ）が好ましい。 The flexible substrate constituting the electrical connection unit (FPC) is not particularly limited as long as it is a transparent and flexible plastic material having sufficient mechanical strength. Polyimide resin (PI), polycarbonate resin, Polyethylene terephthalate resin (PET), polyethylene naphthalate resin (PEN), cycloolefin resin (COP) and the like can be mentioned, and polyimide resin (PI), polyethylene terephthalate resin (PET), polyethylene naphthalate resin (PEN) are preferable. Is preferred.
　表面の回路部と裏面の配線は、導電性を有する金属材料で構成されていることが好ましく、例えば、金、銀、銅、ＩＴＯ等を挙げることができるが、本発明では、銅により形成することが好ましい。 The circuit part on the front surface and the wiring on the back surface are preferably made of a conductive metal material, and examples thereof include gold, silver, copper, and ITO. In the present invention, the wiring is formed of copper. It is preferable.
　透明ＦＰＣと有機ＥＬパネルを電気的に接続する導電性接着剤としては、導電性を備えた部材であれば特に制限はないが、異方性導電膜（ＡＣＦ）、導電性ペースト、又は金属ペーストであることが好ましい態様である。 The conductive adhesive for electrically connecting the transparent FPC and the organic EL panel is not particularly limited as long as it is a member having conductivity, but an anisotropic conductive film (ACF), conductive paste, or metal paste. It is a preferred embodiment.
　異方性導電膜（ＡＣＦ）とは、例えば、熱硬化性樹脂に混ぜ合わせた導電性を持つ微細な導電性粒子を有する層を挙げることができる。本発明に用いることができる導電性粒子含有層としては、異方性導電部材としての導電性粒子を含有する層であれば、特に制限はなく、目的に応じて適宜選択することができる。本発明に係る異方性導電部材として用いることができる導電性粒子としては、例えば、金属粒子、金属被覆樹脂粒子などが挙げられる。市販されているＡＣＦとしては、例えば、ＭＦ－３３１（日立化成製）などの、樹脂フィルムにも適用可能な低温硬化型のＡＣＦを挙げることができる。 Examples of the anisotropic conductive film (ACF) include a layer having fine conductive particles having conductivity mixed with a thermosetting resin. The conductive particle-containing layer that can be used in the present invention is not particularly limited as long as it is a layer containing conductive particles as an anisotropic conductive member, and can be appropriately selected according to the purpose. Examples of the conductive particles that can be used as the anisotropic conductive member according to the present invention include metal particles and metal-coated resin particles. Examples of commercially available ACFs include low-temperature curing ACFs that can also be applied to resin films, such as MF-331 (manufactured by Hitachi Chemical).
　金属粒子としては、例えば、ニッケル、コバルト、銀、銅、金、パラジウムなどが挙げられる。これらは、一種単独で使用してもよいし、二種以上を併用してもよい。これらの中でも、ニッケル、銀、銅が好ましい。これらの表面酸化を防ぐ目的で、表面に金、パラジウムを施した粒子を用いてもよい。更に、表面に金属突起や有機物で絶縁被膜を施したものを用いてもよい。 Examples of the metal particles include nickel, cobalt, silver, copper, gold, and palladium. These may be used individually by 1 type and may use 2 or more types together. Among these, nickel, silver, and copper are preferable. In order to prevent these surface oxidations, particles having gold or palladium on the surface may be used. Furthermore, you may use what gave the metal film and the insulating film with the organic substance on the surface.
　金属被覆樹脂粒子としては、例えば、樹脂コアの表面をニッケル、銅、金、及びパラジウムのいずれかの金属を被覆した粒子が挙げられる。同様に、樹脂コアの最外表面に金、パラジウムを施した粒子を用いてもよい。更に、樹脂コアの表面に金属突起や有機物で絶縁皮膜を施したものを用いてもよい。 Examples of the metal-coated resin particles include particles in which the surface of the resin core is coated with any metal of nickel, copper, gold, and palladium. Similarly, particles obtained by applying gold or palladium to the outermost surface of the resin core may be used. Further, a resin core whose surface is coated with a metal protrusion or an organic material may be used.
　また、金属ペーストとしては、市販されている金属ナノ粒子ペーストである、銀粒子ペースト、銀－パラジウム粒子ペースト、金粒子ペースト、銅粒子ペースト等を適宜選択して用いることができる。金属ペーストとしては、例えば、大研化学社から販売されている有機ＥＬ素子基板用銀ペースト（ＣＡ－６１７８、ＣＡ－６１７８Ｂ、ＣＡ－２５００Ｅ、ＣＡ－２５０３－４、ＣＡ－２５０３Ｎ、ＣＡ－２７１等、比抵抗値：１５～３０ｍΩ・ｃｍ、スクリーン印刷法で形成、硬化温度：１２０～２００℃）、ＬＴＣＣ用ペースト（ＰＡ－８８（Ａｇ）、ＴＣＲ－８８０（Ａｇ）、ＰＡ－Ｐｔ（Ａｇ・Ｐｔ））、ガラス基板用銀ペースト（ＵＳ－２０１、ＵＡ－３０２、焼成温度：４３０～４８０℃）等を挙げることができる。 Further, as the metal paste, a commercially available metal nanoparticle paste, such as a silver particle paste, a silver-palladium particle paste, a gold particle paste, a copper particle paste, or the like, can be appropriately selected and used. Examples of the metal paste include silver pastes for organic EL element substrates (CA-6178, CA-6178B, CA-2500E, CA-2503-4, CA-2503N, CA-271, etc., sold by Daiken Chemical Co., Ltd. , Specific resistance value: 15-30 mΩ · cm, formed by screen printing, curing temperature: 120-200 ° C., LTCC paste (PA-88 (Ag), TCR-880 (Ag), PA-Pt (Ag · Pt)), silver paste for glass substrates (US-201, UA-302, baking temperature: 430 to 480 ° C.), and the like.
　本発明の有機エレクトロルミネッセンスパネルは、輝度均一性を達成し、各種照明装置の面発光体やスマートフォンやタブレット等の各種スマートデバイスに好適に利用できる。 The organic electroluminescence panel of the present invention achieves luminance uniformity and can be suitably used for various smart devices such as surface light emitters of various lighting devices and smartphones and tablets.
　１　基材
　２、１０　ガスバリアー層
　３　陽極（光透過性を有する陽極）
　４　キャリア輸送機能層群１
　５　発光層
　６　キャリア輸送機能層群２
　７　陰極（光透過性を有する陰極）
　８　セパレーター（隔壁）
　９　封止用接着層
　１１　封止基板
　１２　絶縁層
　１３　印加電源
　１４　下地層
　１５　薄膜銀層
　１６　光学調整層
　１７　引出電極
　１８　配線
　１９　ＡＣＦ接続エリア
　２０　ＦＰＣ
　Ｌ　発光光
　ＯＬＥＤ　有機ＥＬ素子
　Ｐ　有機ＥＬパネル
　Ｕ　有機機能層ユニット DESCRIPTION OF SYMBOLS 1 Base material 2, 10 Gas barrier layer 3 Anode (light-transmitting anode)
4 Carrier transport functional layer group 1
5 Light emitting layer 6 Carrier transport functional layer group 2
7 Cathode (Cathode with optical transparency)
8 Separator (partition wall)
9 Sealing Adhesive Layer 11 Sealing Substrate 12 Insulating Layer 13 Applied Power Supply 14 Underlayer 15 Thin Film Silver Layer 16 Optical Adjustment Layer 17 Lead Electrode 18 Wiring 19 ACF Connection Area 20 FPC
L Light emission OLED Organic EL element P Organic EL panel U Organic functional layer unit

Claims (13)

  1. 　非発光時の波長５５０ｎｍにおける光透過率が５０％以上である有機エレクトロルミネッセンス素子を有する有機エレクトロルミネッセンスパネルであって、
    　前記有機エレクトロルミネッセンス素子は、基材上に、少なくとも陽極、有機機能層ユニット及び陰極より構成される発光エリアが、複数に分割されており、
    　前記発光エリアを構成する前記陽極及び前記陰極が、いずれも光透過性を有する電極で構成され、
    　前記陰極が、前記陽極上に設けたセパレーターにより分離した構成であり、
    　かつ、分割されている一方の発光エリアを構成する陽極が、隣接する他方の発光エリアを構成する陰極と、直列に電気的に接続されていることを特徴とする有機エレクトロルミネッセンスパネル。     An organic electroluminescence panel having an organic electroluminescence element having a light transmittance of 50% or more at a wavelength of 550 nm when not emitting light,
    In the organic electroluminescence element, a light emitting area composed of at least an anode, an organic functional layer unit, and a cathode is divided into a plurality of parts on a base material,
    The anode and the cathode constituting the light emitting area are both composed of electrodes having light transmittance,
    The cathode is separated by a separator provided on the anode,
    An organic electroluminescence panel, wherein an anode constituting one of the divided light emitting areas is electrically connected in series with a cathode constituting the other adjacent light emitting area.
  2. 　前記陽極と前記セパレーターとの間に、絶縁層を有することを特徴とする請求項１に記載の有機エレクトロルミネッセンスパネル。 The organic electroluminescence panel according to claim 1, further comprising an insulating layer between the anode and the separator.
  3. 　前記基材が、光透過性を有するガラス基材又はフレキシブル性樹脂基材であることを特徴とする請求項１又は請求項２に記載の有機エレクトロルミネッセンスパネル。 The organic electroluminescence panel according to claim 1 or 2, wherein the base material is a light-transmitting glass base material or a flexible resin base material.
  4. 　前記フレキシブル性樹脂基材が、ガスバリアー層を有していることを特徴とする請求項３に記載の有機エレクトロルミネッセンスパネル。 The organic electroluminescence panel according to claim 3, wherein the flexible resin base material has a gas barrier layer.
  5. 　前記光透過性を有する陽極が、酸化物半導体又は薄膜の金属若しくは合金で構成されていることを特徴とする請求項１から請求項４までのいずれか一項に記載の有機エレクトロルミネッセンスパネル。 The organic electroluminescence panel according to any one of claims 1 to 4, wherein the light-transmitting anode is made of an oxide semiconductor, a thin-film metal, or an alloy.
  6. 　前記光透過性を有する陰極が、少なくとも薄膜の金属又は合金で構成されていることを特徴とする請求項１から請求項５までのいずれか一項に記載の有機エレクトロルミネッセンスパネル。 6. The organic electroluminescence panel according to claim 1, wherein the light-transmitting cathode is made of at least a thin-film metal or alloy.
  7. 　前記光透過性を有する陰極が、含窒素化合物を用いて構成された下地層と、当該下地層上に、銀又は銀を主成分とした合金で構成されている電極層を有する構成であることを特徴とする請求項１から請求項６までのいずれか一項に記載の有機エレクトロルミネッセンスパネル。 The light-transmitting cathode has an underlayer composed of a nitrogen-containing compound and an electrode layer composed of silver or an alloy containing silver as a main component on the underlayer. The organic electroluminescence panel according to any one of claims 1 to 6, wherein
  8. 　前記有機エレクトロルミネッセンスパネルと外部電極との接続部は、導電性接着剤により電気的接続されていることを特徴とする請求項１から請求項７までのいずれか一項に記載の有機エレクトロルミネッセンスパネル。 The organic electroluminescence panel according to any one of claims 1 to 7, wherein a connection portion between the organic electroluminescence panel and the external electrode is electrically connected by a conductive adhesive. .
  9. 　前記複数の有機エレクトロルミネッセンス素子が、ガスバリアー層を有するフレキシブル性樹脂部材により封止されていることを特徴とする請求項１から請求項８までのいずれか一項に記載の有機エレクトロルミネッセンスパネル。 The organic electroluminescence panel according to any one of claims 1 to 8, wherein the plurality of organic electroluminescence elements are sealed with a flexible resin member having a gas barrier layer.
  10. 　前記複数の発光エリアが、前記セパレーターにより分離され、ストライプ状に並列配置されていることを特徴とする請求項１から請求項９までのいずれか一項に記載の有機エレクトロルミネッセンスパネル。 The organic electroluminescence panel according to any one of claims 1 to 9, wherein the plurality of light emitting areas are separated by the separator and arranged in parallel in a stripe shape.
  11. 　前記外部電極は、光透過性を有するフレキシブルプリント回路から構成されることを特徴とする請求項８から請求項１０までのいずれか一項に記載の有機エレクトロルミネッセンスパネル。 The organic electroluminescence panel according to any one of claims 8 to 10, wherein the external electrode is composed of a flexible printed circuit having optical transparency.
  12. 　請求項１から請求項１１までのいずれか一項に記載の有機エレクトロルミネッセンスパネルを製造する有機エレクトロルミネッセンスパネルの製造方法であって、
    　非発光時の波長５５０ｎｍにおける光透過率が５０％以上である有機エレクトロルミネッセンス素子を有し、
    　当該有機エレクトロルミネッセンス素子において、基材上に、少なくとも陽極、有機機能層ユニット及び陰極より構成される発光エリアを、複数に分割して形成し、
    　前記陰極を、前記陽極上に設けたセパレーターにより分離したパターンを形成し、
    　分割されている一方の発光エリアを構成する陽極を、隣接する他方の発光エリアを構成する陰極と、直列に電気的に接続し、
    　かつ、前記陽極、陰極及びセパレーターを、フォトリソグラフィー法により形成することを特徴とする有機エレクトロルミネッセンスパネルの製造方法。     It is a manufacturing method of the organic electroluminescent panel which manufactures the organic electroluminescent panel as described in any one of Claim 1- Claim 11,
    Having an organic electroluminescence device having a light transmittance of 50% or more at a wavelength of 550 nm when not emitting light,
    In the organic electroluminescence element, on the base material, a light emitting area composed of at least an anode, an organic functional layer unit and a cathode is divided into a plurality of parts,
    Forming a pattern in which the cathode is separated by a separator provided on the anode;
    The anode constituting one light emitting area that is divided is electrically connected in series with the cathode constituting the other neighboring light emitting area,
    And the said anode, a cathode, and a separator are formed by the photolithographic method, The manufacturing method of the organic electroluminescent panel characterized by the above-mentioned.
  13. 　前記陽極と前記セパレーターとの間に、フォトリソグラフィー法を用いて絶縁層を形成することを特徴とする請求項１２に記載の有機エレクトロルミネッセンスパネルの製造方法。 13. The method of manufacturing an organic electroluminescence panel according to claim 12, wherein an insulating layer is formed between the anode and the separator using a photolithography method.
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